Composition of matter tailoring: system I

ABSTRACT

The present invention relates to new compositions of matter, particularly metals and alloys, and methods of making such compositions. The new compositions of matter exhibit long-range ordering and unique electronic character.

RELATED APPLICATIONS

This application is a divisional of U.S. Ser. No. 10/123,028, filed Apr.12, 2002, now U.S. Pat. No. 6,921,497, issued Jul. 26, 2005, which is acontinuation-in-part of U.S. Ser. No. 09/416,720, filed Oct. 13, 1999,now U.S. Pat. No. 6,572,792, issued Jun. 3, 2003, and acontinuation-in-part of International Application No. PCT/US00/28549,which designated the United States and was filed on Oct. 13, 2000,published in English, which is a continuation of U.S. Ser. No.09/416,720, filed Oct. 13, 1999, now U.S. Pat. No. 6,572,792, issuedJun. 3, 2003. The entire teachings of the above applications areincorporated herein by reference.

BACKGROUND OF THE INVENTION

All matter has structure. The structure of matter emanates from theelectronic structure of the elements of the periodic table. It is theelectronic structure of the elements and the new electronic structuresthat arise as a consequence of their combination in molecules thatdefine the electronic state and character of matter. It is also theelectronic structure that creates the properties identified andassociated with elements and the matter that results from theircombination and arrangement (e.g., molecules and matter).

Certain combinations of elements give rise to states of matter withparticularly desirable properties. For instance, certain states ofmatter have long-range order, which refers to matter that has repeatingaligned chemical, electronic, or structural units. Example of suchstates of matter include surfactant membranes, crystals such as smecticliquid crystals and liquid crystalline polymers, and magnetic materials.

One means of imparting unique properties to a material involves addingcarbon to the material. Depending on the parent material and on theamount of carbon added, carbon may remain dissolved in a material or mayprecipitate out to form discrete carbon structures.

SUMMARY OF THE INVENTION

The present invention relates to a new composition of matter comprisedof ‘p’, ‘d’, and/or ‘f’ atomic orbitals, and a process for making thecomposition of matter. This new composition of matter can bedistinguished by a change in energy, electronic properties, physicalproperties, and the like. X-ray fluorescence spectroscopy is a preferredmethod of detecting and distinguishing new compositions of matter. Thechange in properties can be controlled to be transient, fixed, oradjustable (temporarily permanent) and includes properties such asmechanical, electrical, chemical, thermal, engineering, and physicalproperties, as well structural character of the composition of matter(e.g., alignment, orientation, order, anisotropy, and the like).

The present invention includes manufactured metals and alloyscharacterized by the x-ray fluorescence spectrometry plots and elementalabundance tables (obtained from x-ray fluorescence analysis) containedherein.

The present invention is additionally a method of processing a metal oran alloy of metals, comprising the steps of:

-   -   (A.) adding the metal or alloy to a reactor in one or more steps        and melting said metal or alloy;    -   (B.) adding a carbon source to the molten metal or alloy and        dissolving carbon in said molten metal or alloy, followed by        removing the undissolved carbon source;    -   (C.) increasing the temperature of the molten metal or alloy;    -   (D.) varying the temperature of the molten metal or alloy        between two temperatures over one or more cycles;    -   (E.) adding a flow of an inert gas through the molten metal or        alloy;    -   (F.) varying the temperature of the molten metal or alloy        between two temperatures over one or more cycles;    -   (G.) adding a carbon source to the molten metal or alloy and        further dissolving carbon in said molten metal or alloy,        followed by removing the undissolved carbon source;    -   (H.) varying the temperature of the molten metal or alloy        between two temperatures over one or more cycles, wherein the        molten metal or alloy has a greater degree of saturation with        carbon than in Step (F.);    -   (I.) stopping the flow of the inert gas;    -   (J.) varying the temperature of the molten metal or alloy        between two temperatures over one or more cycles, wherein the        molten metal or alloy has a greater degree of saturation with        carbon than in Step (H.) and wherein an inert gas is added as        the temperature is lowered and an inert gas, chosen        independently, is added as the temperature is raised;    -   (K.) varying the temperature of the molten metal or alloy        between two temperatures over one or more cycles, wherein the        molten metal or alloy has a greater degree of saturation with        carbon than in Step (J.) and wherein an inert gas is added as        the temperature is lowered and an inert gas, chosen        independently, is added as the temperature is raised;    -   (L.) stopping the flow of the inert gases;    -   (M.) varying the temperature of the molten metal or alloy        between two temperatures over one or more cycles, wherein the        molten metal or alloy has an equal or greater degree of        saturation with carbon than in Step (K.); and    -   (N.) cooling the molten metal or alloy to room temperature,        thereby obtaining a solidified manufactured metal or alloy.

Steps (D.), (F.), (H.), (J.), (K.), and (L.) of the present method arecommonly referred to as “cycling steps” below. For purposes of thepresent invention, carbon “dissolved” in a metal is defined as carbonthat has been solubilized in a molten metal, adsorbed by a metal,reacted with a metal, or has otherwise interacted with a metal such thatcarbon is desorbed or transferred from a solid carbon source into amolten metal.

Preferably, the present invention is a method of processing copper,comprised of the steps described above.

The present invention also includes a method of processing a metal or analloy of metals, comprising the steps of:

-   -   (A.) adding the metal or alloy to a reactor in one or more steps        and melting said metal or alloy;    -   (B.) adding a carbon source to the molten metal or alloy and        dissolving carbon in said molten metal or alloy, followed by        removing the undissolved carbon source;    -   (C.) varying the temperature of the molten metal or alloy        between two temperatures over two or more cycles;    -   (D.) adding a carbon source to the molten metal or alloy and        further dissolving carbon in said molten metal or alloy,        followed by removing the undissolved carbon source;    -   (E.) varying the temperature of the molten metal or alloy        between two temperatures over two or more cycles, wherein the        molten metal or alloy has a greater degree of saturation with        carbon than in Step (D.); and    -   (F.) cooling the molten metal or alloy to room temperature,        thereby obtaining a solidified manufactured metal or alloy;

further characterized by adding a flow of inert gas, before, during, orafter one or more of Steps (B.) through (E.).

In another embodiment, the present invention is a method of processingcopper, or other metal or alloy comprising:

-   -   (1.) contacting molten copper or other metal or alloy with a        carbon source;    -   (2.) an iterative cycling process, wherein relative saturation        of copper or other metal or alloy with carbon remains the same        or increases independently with each cycle; and    -   (3.) cooling the molten copper or other metal or alloy to room        temperature, thereby obtaining a solidified manufactured copper        or other metal or alloy.

Advantages of the present invention include a method of processingmetals into new compositions of matter and producing and characterizingcompositions of matter with altered physical and/or electricalproperties.

BRIEF DESCRIPTION OF THE DRAWINGS

FIGS. 1A and 1B show non-contact magnetic force microscopy images ofnatural copper and manufactured copper, respectively.

FIG. 2A shows non-contact magnetic force microscopy of manufacturedcopper.

FIG. 2B shows scanning tunneling microscopy images of manufacturedcopper.

FIGS. 3A, 3B, and 4A and 4B show x-ray emission spectrometry images ofnatural copper and manufactured copper.

FIG. 5A shows a non-contact magnetic force microscopy image ofmanufactured copper. FIG. 5B shows a x-ray emission spectroscopy imageof manufactured copper.

FIGS. 6A and 6B show a plot of an x-ray fluorescence spectrometrycomparison of manufactured copper and natural copper.

FIG. 7 shows a plot of an X-ray fluorescence spectrometry in relation tothe direction of the scan.

FIG. 8 shows a plot of a change in capacitance and voltage decay for amanufactured metal.

FIG. 9 shows a plot of a change in voltage gradients for a moltenmanufactured metal as the position of an electrode within the melt ischanged.

FIG. 10 shows a plot of the observed voltage of a manufacturedcopper-nickel alloy, as measured in a molten state.

FIG. 11 shows a plot of the observed voltage of a manufactured metal, asmeasured in a molten state.

FIG. 12 shows a plot of a positive voltage signature and positivecapacitance decay of a manufactured metal, as measured in a moltenstate.

FIG. 13 shows a plot of a voltage decay profile of a manufactured metal,as measured in a molten state.

FIG. 14 shows a plot of a neutral decay in voltage and capacitance, asmeasured in a molten state.

FIG. 15 shows a plot of a positive voltage signature and a negativecapacitance decay of a manufactured metal, as measured in a moltenstate.

FIG. 16 shows a plot of the voltage over time of a manufactured metalunder pressure.

FIGS. 17A, 17B, 17C, 18A, 18B and 18C show optical and scanning electronmicroscopy images of manufactured copper.

FIGS. 19A, 19B, 20A and 20B show optical microscopy images ofmanufactured nickel.

FIGS. 21A, 21B and 21C show images of atomic force microscopy andscanning tunneling microscopy of manufactured copper from an axialanalysis.

FIGS. 22A, 22B and 22C show images of atomic force microscopy andnon-contact magnetic force microscopy of manufactured copper from aradial analysis.

FIGS. 23A, 23B and 23C show images of discrete induced magnetism ofnon-magnetic copper.

FIG. 24 shows a plot of electrical susceptance for manufacturedcompositions in comparison to the compositions in its natural state.

FIG. 25 shows a plot of x-ray fluorescence spectrometry for manufacturedcopper, on both the axial and radial faces of a block cut from the ingotprepared in Example 1, as compared to a plot of x-ray fluorescencespectrometry for natural copper.

FIG. 26 shows a plot of x-ray fluorescence spectrometry for manufacturedcopper in the region of the K_(α) band of aluminum, on the bottom faceof a block cut from the ingot prepared in Example 1, as compared to aplot of x-ray fluorescence spectrometry for natural aluminum.

FIGS. 27A and 27B show plots of x-ray fluorescence spectrometry formanufactured nickel, on both the axial and radial faces of a block cutfrom the ingot prepared in Example 2, as compared to plots of x-rayfluorescence spectrometry for natural nickel.

FIG. 28A shows a plot of x-ray fluorescence spectrometry formanufactured nickel in the region of the K_(α) band of aluminum, on theaxial and radial faces of a block cut from the ingot prepared in Example2, as compared to a plot of x-ray fluorescence spectrometry for naturalaluminum.

FIG. 28B shows a plot of x-ray fluorescence spectrometry formanufactured nickel in the region of the K_(α) band of zirconium, on theaxial and radial faces of a block cut from the ingot prepared in Example2, as compared to a plot of x-ray fluorescence spectrometry for naturalzirconium.

FIG. 29 shows a plot of x-ray fluorescence spectrometry for manufacturednickel in the region of the K_(α) band of sulfur, on all six faces of ablock cut from the ingot prepared in Example 2, as compared to a plot ofx-ray fluorescence spectrometry for natural sulfur.

FIG. 30 shows a plot of x-ray fluorescence spectrometry for manufacturednickel in the region of the K_(α) band of chlorine (from potassiumchloride), on the axial and radial faces of a block cut from the ingotprepared in Example 2, as compared to a plot of x-ray fluorescencespectrometry for natural chlorine (from potassium chloride).

FIGS. 31A and 31B show plots of x-ray fluorescence spectrometry formanufactured cobalt, on both the axial and radial faces of a block cutfrom the ingot prepared in Example 3, as compared to plots of x-rayfluorescence spectrometry for natural cobalt.

FIG. 32A shows a plot of x-ray fluorescence spectrometry formanufactured cobalt in the region of the K_(α) band of aluminum, on theaxial and radial faces of a block cut from the ingot prepared in Example3, as compared to a plot of x-ray fluorescence spectrometry for naturalaluminum.

FIG. 32B shows a plot of x-ray fluorescence spectrometry formanufactured cobalt in the region of the K_(α) band of iron, on theaxial and radial faces of a block cut from the ingot prepared in Example3, as compared to a plot of x-ray fluorescence spectrometry for naturaliron.

FIG. 33A shows a plot of x-ray fluorescence spectrometry formanufactured cobalt in the region of the K_(α) band of chlorine (frompotassium chloride), on the axial and radial faces of a block cut fromthe ingot prepared in Example 3, as compared to a plot of x-rayfluorescence spectrometry for natural chlorine (from potassiumchloride).

FIG. 33B shows a plot of x-ray fluorescence spectrometry formanufactured cobalt in the region of the K_(α) band of zirconium, on theaxial and radial faces of a block cut from the ingot prepared in Example3, as compared to a plot of x-ray fluorescence spectrometry for naturalzirconium.

FIG. 34 shows a plot of x-ray fluorescence spectrometry for manufacturedcobalt in the region of the K_(α) band of manganese, on the axial andradial faces of a block cut from the ingot prepared in Example 3, ascompared to a plot of x-ray fluorescence spectrometry for naturalmanganese.

FIG. 35 shows a plot of x-ray fluorescence spectrometry for amanufactured copper/silver/gold alloy in the region of the K_(α) band ofcopper, on the axial and radial faces of a block cut from the ingotprepared in Example 4, as compared to a plot of x-ray fluorescencespectrometry for natural copper.

FIG. 36 shows a plot of x-ray fluorescence spectrometry for amanufactured copper/silver/gold alloy in the region of the K_(α) band ofgold, on the axial and radial faces of a block cut from the ingotprepared in Example 4, as compared to a plot of x-ray fluorescencespectrometry for natural silver.

FIG. 37 shows a plot of x-ray fluorescence spectrometry for amanufactured copper/silver/gold alloy in the region of the K_(α) band ofsilver, on the axial and radial faces of a block cut from the ingotprepared in Example 4, as compared to a plot of x-ray fluorescencespectrometry for natural gold.

FIG. 38 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/lead/zinc alloy in the region of the K_(α) band of tin,on the axial and radial faces of a block cut from the ingot prepared inExample 5, as compared to a plot of x-ray fluorescence spectrometry fornatural tin.

FIG. 39 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/lead/zinc alloy in the region of the K_(α) band ofzinc, on the axial and radial faces of a block cut from the ingotprepared in Example 5, as compared to a plot of x-ray fluorescencespectrometry for natural zinc.

FIG. 40 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/lead/zinc alloy in the region of the K_(α) band oflead, on the axial and radial faces of a block cut from the ingotprepared in Example 5, as compared to a plot of x-ray fluorescencespectrometry for natural lead.

FIG. 41 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/sodium/magnesium/potassium alloy in the region of theK_(α) band of potassium (from potassium chloride), on the axial andradial faces of a block cut from the ingot prepared in Example 6, ascompared to a plot of x-ray fluorescence spectrometry for naturalpotassium (from potassium chloride).

FIG. 42 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/sodium/magnesium/potassium alloy in the region of theK_(α) band of tin, on the axial and radial faces of a block cut from theingot prepared in Example 6, as compared to a plot of x-ray fluorescencespectrometry for natural tin.

FIG. 43 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/sodium/magnesium/potassium alloy in the region of theK_(α) band of magnesium (using magnesium oxide), on the axial and radialfaces of a block cut from the ingot prepared in Example 6, as comparedto a plot of x-ray fluorescence spectrometry for natural magnesium(using magnesium oxide).

FIG. 44 shows a plot of x-ray fluorescence spectrometry for amanufactured tin/sodium/magnesium/potassium alloy in the region of theK_(α) band of sodium (using AlNa₃F₆), on the axial and radial faces of ablock cut from the ingot prepared in Example 6, as compared to a plot ofx-ray fluorescence spectrometry for natural sodium (using AlNa₃F₆).

FIGS. 45A and 45B show plots of x-ray fluorescence spectrometry formanufactured silicon, on both the axial and radial faces of a block cutfrom the ingot prepared in Example 7, as compared to plots of x-rayfluorescence spectrometry for natural silicon.

FIG. 46A shows a plot of x-ray fluorescence spectrometry formanufactured silicon in the region of the K_(α) band of aluminum, on theaxial and radial faces of a block cut from the ingot prepared in Example7, as compared to a plot of x-ray fluorescence spectrometry for naturalaluminum.

FIG. 46B shows a plot of x-ray fluorescence spectrometry formanufactured silicon in the region of the K_(α) band of titanium, on theaxial and radial faces of a block cut from the ingot prepared in Example7, as compared to a plot of x-ray fluorescence spectrometry for naturaltitanium.

FIG. 47A shows a plot of x-ray fluorescence spectrometry formanufactured silicon in the region of the K_(α) band of sulfur, on theaxial and radial faces of a block cut from the ingot prepared in Example7, as compared to a plot of x-ray fluorescence spectrometry for naturalsulfur.

FIG. 47B shows a plot of x-ray fluorescence spectrometry formanufactured silicon in the region of the K_(α) band of chlorine (frompotassium chloride), on the axial and radial faces of a block cut fromthe ingot prepared in Example 7, as compared to a plot of x-rayfluorescence spectrometry for natural chlorine (from potassiumchloride).

FIG. 48A shows a plot of x-ray fluorescence spectrometry formanufactured silicon in the region of the K_(α) band of gallium (fromgallium oxide), on the axial and radial faces of a block cut from theingot prepared in Example 7, as compared to a plot of x-ray fluorescencespectrometry for natural gallium (from gallium oxide).

FIG. 48B shows a plot of x-ray fluorescence spectrometry formanufactured silicon in the region of the K_(α) band of potassium (frompotassium chloride), on the axial and radial faces of a block cut fromthe ingot prepared in Example 7, as compared to a plot of x-rayfluorescence spectrometry for natural potassium (from potassiumchloride).

FIGS. 49A and 49B show plots of x-ray fluorescence spectrometry formanufactured iron, on both the axial and radial faces of a block cutfrom the ingot prepared in Example 8, as compared to plots of x-rayfluorescence spectrometry for natural iron.

FIG. 50A shows a plot of x-ray fluorescence spectrometry formanufactured iron in the region of the K_(α) band of aluminum, on theaxial and radial faces of a block cut from the ingot prepared in Example8, as compared to a plot of x-ray fluorescence spectrometry for naturalaluminum.

FIG. 50B shows a plot of x-ray fluorescence spectrometry formanufactured iron in the region of the K_(α) band of zirconium, on theaxial and radial faces of a block cut from the ingot prepared in Example8, as compared to a plot of x-ray fluorescence spectrometry for naturalzirconium.

FIG. 51A shows a plot of x-ray fluorescence spectrometry formanufactured iron in the region of the K_(α) band of sulfur, on theaxial and radial faces of a block cut from the ingot prepared in Example8, as compared to a plot of x-ray fluorescence spectrometry for naturalsulfur.

FIG. 51B shows a plot of x-ray fluorescence spectrometry formanufactured iron in the region of the K_(α) band of chlorine (frompotassium chloride), on the axial and radial faces of a block cut fromthe ingot prepared in Example 8, as compared to a plot of x-rayfluorescence spectrometry for natural chlorine (from potassiumchloride).

FIG. 52 shows a plot of x-ray fluorescence spectrometry for amanufactured iron/vanadium/chromium/manganese alloy in the region of theK_(α) band of chromium (using chromium(III) oxide), on the axial andradial faces of a block cut from the ingot prepared in Example 9, ascompared to a plot of x-ray fluorescence spectrometry for naturalchromium (using chromium (III) oxide).

FIG. 53 shows a plot of x-ray fluorescence spectrometry for amanufactured iron/vanadium/chromium/manganese alloy in the region of theK_(α) band of iron, on the axial and radial faces of a block cut fromthe ingot prepared in Example 9, as compared to a plot of x-rayfluorescence spectrometry for natural iron.

FIG. 54 shows a plot of x-ray fluorescence spectrometry for amanufactured iron/vanadium/chromium/manganese alloy in the region of theK_(α) band of vanadium, on the axial and radial faces of a block cutfrom the ingot prepared in Example 9, as compared to a plot of x-rayfluorescence spectrometry for natural vanadium.

FIG. 55 shows a plot of x-ray fluorescence spectrometry for amanufactured iron/vanadium/chromium/manganese alloy in the region of theK_(α) band of manganese, on the axial and radial faces of a block cutfrom the ingot prepared in Example 9, as compared to a plot of x-rayfluorescence spectrometry for natural manganese.

FIG. 56 shows a plot of x-ray fluorescence spectrometry for amanufactured iron/vanadium/chromium/manganese alloy in the region of theK_(α) band of sulfur, on all six sides of a block cut from the ingotprepared in Example 9.

FIG. 57 shows a plot of x-ray fluorescence spectrometry for amanufactured nickel/tantalum/hafnium/tungsten alloy in the region of theK_(α) band of tantalum, on the axial and radial faces of a block cutfrom the ingot prepared in Example 10, as compared to a plot of x-rayfluorescence spectrometry for natural tantalum.

FIG. 58 shows a plot of x-ray fluorescence spectrometry for amanufactured nickel/tantalum/hafnium/tungsten alloy in the region of theK_(α) band of tungsten, on the axial and radial faces of a block cutfrom the ingot prepared in Example 10, as compared to a plot of x-rayfluorescence spectrometry for natural tungsten.

FIG. 59 shows a plot of x-ray fluorescence spectrometry for amanufactured nickel/tantalum/hafnium/tungsten alloy in the region of theK_(α) band of hafnium, on the axial and radial faces of a block cut fromthe ingot prepared in Example 10, as compared to a plot of x-rayfluorescence spectrometry for natural hafnium.

FIG. 60 shows a plot of x-ray fluorescence spectrometry for amanufactured nickel/tantalum/hafnium/tungsten alloy in the region of theK_(α) band of sulfur, on all six faces of a block cut from the ingotprepared in Example 10.

FIG. 61 shows a plot of x-ray fluorescence spectrometry for amanufactured nickel/tantalum/hafnium/tungsten alloy in the region of theK_(α) band of nickel, on the axial and radial faces of a block cut fromthe ingot prepared in Example 10, as compared to a plot of x-rayfluorescence spectrometry for natural nickel.

FIG. 62 shows the general configuration of the ARL 8410 spectrometer.

DETAILED DESCRIPTION OF THE INVENTION

Electromagnetic chemistry is the science that affects the transfer andcirculation of energy in many forms when induced by changes inelectromagnetic energy. The theory of Electrodynamics of Moving Bodies(Einstein, 1905) mandates that when the electrodynamic components of thematerial are manipulated, changes in the energy levels within the atomicorbitals must be induced. These changes in the atomic orbitals are thevehicles by which changes in the (material) properties, such as themagnitude and/or the orientation, can occur. Alignment of theelectrodynamic component induces effects that may result in significantchanges in the underlying material species: (1) alignment of atoms withthe resulting directionality of physical properties; (2) alignment ofenergy levels and the capability to produce harmonics, may establishphysical properties conducive for energy transfer; (3) alignment of theelectrodynamic component include the opening of pathways for freeelectron flow, and; (4) alignment of electrodynamic field phaseorientation.

The present invention relates to new compositions of matter, referred toherein as “manufactured” metals or alloys of metals. A “manufactured”metal or alloy is a metal or alloy which exhibits a change in electronicstructure, such as that seen in a fluid XRF spectrum. The AmericanHeritage College Dictionary, Third Edition defines “fluid” as changingor tending to change.

Metals of the present invention are generally p, d, or f block metals.Metals include transition metals such as Group 3 metals (e.g., scandium,yttrium, lanthanum), Group 4 metals (e.g, titanium, zirconium, hafnium),Group 5 metals (vanadium, niobium, tantalum), Group 6 metals (e.g.,chromium, molybdenum, tungsten), Group 7 metals (e.g., manganese,technetium, rhenium), Group 8 metals (e.g., iron, ruthenium, osmium),Group 9 metals (e.g., cobalt, rhodium, iridium), Group 10 metals(nickel, palladium, platinum), Group 11 metals (e.g., copper, silver,gold), and Group 12 metals (e.g., zinc, cadmium, mercury). Metals of thepresent invention also include alkali metals (e.g., lithium, sodium,potassium, rubidium, cesium) and alkaline earth metals (e.g., berylliummagnesium, calcium, strontium, barium). Additional metals includealuminum, gallium, indium, tin, lead, boron, germanium, arsenic,antimony, tellurium, bismuth, and silicon.

The present invention also includes alloys of metals. Alloys aretypically mixtures of metals. Alloys of the present invention can beformed, for example, by melting together two or more of the metalslisted above. Preferred alloys include those comprised of copper, gold,and silver; tin, zinc, and lead; tin, sodium, magnesium, and potassium;iron, vanadium, chromium, and manganese; and nickel, tantalum, hafnium,and tungsten.

Carbon sources of the present invention include materials that arepartially, primarily, or totally comprised of carbon. Those carbonsources that are non-organic and comprised partially of carbon areprimarily comprised of one or more metals. Suitable carbon sourcesinclude graphite rods, graphite powder, graphite flakes, fullerenes,diamonds, natural gas, methane, ethane, propane, butane, pentane, castiron, iron comprising carbon, steel comprising carbon, and combinationsthereof. A preferred carbon source is a high purity (<5 ppm impurities)carbon source. Another preferred carbon source is a high purity (<5 ppmimpurities) graphite rod. The carbon source is selected, in part, basedon the system to which it is added. In one example, graphite rods andgraphite flakes are added to copper, typically in a sequential manner.In another example, graphite rods and graphite powder are added to iron,typically in a sequential manner.

Carbon sources can be contacted with molten metals for variable periodsof time. The period of time the carbon source is in contact with moltenmetals is the time between adding the carbon source and removing theundissolved carbon source. The period of time can be from about 0.5hours to about 12 hours, about 1 hour to about 10 hours, about 2 hoursto about 8 hours, about 3 hours to about 6 hours, about 3.5 hours toabout 4.5 hours, or about 3.9 hours to about 4.1 hours. Alternatively,the period of time can be from about 5 minutes to about 300 minutes,about 10 minutes to about 200 minutes, about 20 minutes to about 120minutes, about 30 minutes to about 90 minutes, about 40 minutes to about80 minutes, about 50 minutes to about 70 minutes, or about 59 minutes toabout 61 minutes.

A cycle of the present invention includes a period of time where thetemperature and/or the degree to which a metal is saturated with carbonis varied. Over a period of time, varying the temperature involves aperiod of raising (or increasing) the temperature of a metal or alloyand a period when the temperature of a metal or alloy decreases (eitherpassively, such as by heat transfer to the surrounding environment, oractively, such as by mechanical means), in any order. Inert gas can beadded during a cycle, except where it is specified that inert gasaddition is ceased prior to that cycle. Increasing the temperature ofthe metal or alloy increases the amount of carbon that can be dissolvedinto that metal or alloy, which therefore decreases the degree to whichthe metal or alloy is saturated with carbon (relative to the temperatureand degree of carbon saturation when graphite saturation assemblies areremoved the first time). Similarly, decreasing the temperature of themetal or alloy increases the (relative) degree to which the metal oralloy is saturated with carbon.

The degree to which a metal is saturated with carbon varies over thecourse of a method, as well as within each step. In Examples 1-14, thedegree of carbon saturation varies between 70% and 95% in the firstcycling step, between 70% and 95% in the second cycling step, between101% and 103% in the third cycling step, between 104% and 107% in thefourth cycling step, between 108% and 118% in the fifth cycling step,and between 114% and 118% in the sixth cycling step. The cycling stepscorrespond to Steps (D.), (F.), (H.), (J.), (K.), and (L.),respectively, of the method described in the third paragraph of thesummary.

One example of a method of the present invention can be described interms of carbon saturation values. After a metal or alloy is added to asuitable reactor, establish the dissolved carbon level at 70% to 95% ofthe equilibrium saturation of carbon for the thermodynamic statespecified (e.g., T, P, composition) when the composition is in itsnatural state (hereinafter the equilibrium saturation of carbon isreferred to as “[C]_(eqsat)”). Identify temperature set points for 80%and 95% [C]_(eqsat). Vary the temperature between the predetermined setpoints, such that the temperature is decreased for 7 minutes andincreased over 7 minutes per cycle, for 15 cycles. Next, establish aflow of argon. Vary the temperature between the predetermined setpoints, such that the temperature is decreased for 7 minutes andincreased over 7 minutes per cycle, for 5 cycles; the temperature shouldbe maintained above 70% [C]_(eqsat) at all times and maintained below95% [C]_(eqsat) at all times. The carbon level is raised to saturation(i.e., [C]_(eqsat)) with continued argon addition. Hold for 60 minutesat saturation (i.e., [C]_(eqsat)) with continued argon addition. Raisethe carbon level to ⁺1%_(wt) (i.e., ⁺1%_(wt) represents 1%_(wt) abovethe saturation value as defined in its natural state) of [C]_(eqsat)with continued argon addition and hold for 5 minutes. Vary thetemperature for 20 cycles to remain between ⁺1%_(wt) and ⁺3%_(wt) of[C]_(eqsat), such that the temperature is decreased over 9 minutes andincreased over 9 minutes per cycle. Cease argon addition. Cool the metalto ⁺4%_(wt) of [C]_(eqsat). Vary the temperature for 4.5 cycles toremain between ⁺4%_(wt) and ⁺7%_(wt) of [C]_(eqsat), such that thetemperature is decreased over 3 minutes and increased over 5 minutes.Argon is added as the carbon saturation increases and nitrogen is addedas carbon saturation decreases. Cool the metal to obtain ⁺8%_(wt) withcontinued argon addition. Vary the temperature over 15.5 cycles toremain between ⁺8%_(wt) and ⁺18%_(wt) of [C]_(eqsat), such that thetemperature is decreased over 15 minutes and increased over 15 minutes.Argon is added as the carbon saturation increases and nitrogen is addedas carbon saturation decreases. After the 15.5 cycles are complete, gasaddition is halted. Perform one complete cycle by varying thetemperature to remain between ⁺18%_(wt) to ⁺14%_(wt) of [C]_(eqsat)(ending at ⁺18%_(wt)), such that the temperature is increased over 15minutes and decreased over 15 minutes. Proceed immediately to a cooldown that leads to solidification.

An iterative cycle process is a process comprising two or more cycles,whereby one or more of the cycles are carried out at a temperature belowthe carbon saturation point and one or more cycles are carried out at atemperature above the carbon saturation point. For example, in Example1, the first cycle is carried out between 2480° F. and 2530° F., thesecond cycle is carried out between 2480° F. and 2530° F., the thirdcycle is carried out at 2453° F. and 2459° F., the fourth cycle iscarried out between 2441° F. and 2450° F., the fifth cycle is carriedout between 2406° F. and 2438° F., and the sixth cycle is carried outbetween 2406° F. and 2419° F. A cycle following an earlier cycle canhave the identical temperature range as the earlier cycle, a partiallyoverlapping temperature range with the earlier cycle, a temperaturerange above that of the earlier cycle, or a temperature cycle below thatof the earlier cycle. Partially overlapping temperature ranges includesranges where one temperature range falls within the limits of a secondtemperature range (e.g., 2406° F. to 2438° F. and 2406° F. to 2419° F.).Preferably, during an iterative cycling process, the degree to which themetal or alloy is saturated with carbon increases over the process.

Cycles of the present invention can vary in duration. The duration of acycle can vary among cycles in a step. A cycle duration is, for example,about 2 minutes to about 90 minutes, about 3 minutes to about 67minutes, about 5 minutes to about 45 minutes, about 8 minutes to about30 minutes, about 10 minutes to about 20 minutes, about 14 minutes toabout 18 minutes, about 7 minutes to about 9 minutes, about 13 minutesto about 15 minutes, about 17 minutes to about 19 minutes, about 28minutes to about 32 minutes, or about 29 minutes to about 31 minutes.

A cycle can be symmetry or asymmetric. In a symmetric cycle, the periodof increasing the metal or alloy temperature is equal to the period ofdecreasing the metal or alloy temperature. In an asymmetric cycle, theperiod of increasing the metal or alloy temperature is different thanthe period of decreasing the metal or alloy temperature. For anasymmetric cycle, the period of increasing the metal or alloytemperature can be longer than or shorter than the period of decreasingthe metal or alloy temperature.

For example, in a cycle lasting about 7 minutes to about 9 minutes, thetemperature can be increased for about 3 minutes and the temperature canbe decreased for about 5 minutes. If the cycle lasts about 13 minutes toabout 15 minutes, the temperature can be increased for about 7 minutesand the temperature can be decreased for about 7 minutes. If the cyclelasts about 17 minutes to about 19 minutes, the temperature can beincreased for about 9 minutes and the temperature can be decreased forabout 9 minutes. If the cycle lasts about 29 minutes to about 31minutes, the temperature can be increased for about 15 minutes and thetemperature can decreased for about 15 minutes.

The number of cycles in a step is generally an integer or half-integervalue. For example, the number of cycles in a step can be one or more,one to forty, or one to twenty. The number of cycles can be 1, 2, 3, 4,5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23,24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, or 40.Alternatively, the number of cycles in a step can be 0.5, 1.5, 2.5, 3.5,4.5, 5.5, 6.5, 7.5, 8.5, 9.5, 10.5, 11.5, 12.5, 13.5, 14.5, 15.5, 16.5,17.5, 18.5, 19.5, 20.5, 21.5, 22.5, 23.5, 24.5, 25.5, 26.5, 27.5, 28.5,29.5, or 30.5. In a step comprising a half-integer or a non-integerquantity of cycles, either heating or cooling can occur first.

After the initial heating step, the temperature of a metal or an alloyis sufficiently high, such that the temperature is equal to or greaterthan the solidus temperature. The solidus temperature varies dependingon the metal or the alloy, and the amount of carbon dissolved therein.The temperature at the end of Step (F.) of the third paragraph of thesummary is typically about 900° F. to about 3000° F., but varies frommetal to metal. For example, the temperature at the end of Step (F.) canbe about 1932° F. to about 2032° F., about 1957° F. to about 2007° F.,or about 1932° F. to about 2467° F. for copper; about 2368° F. to about2468° F., about 2393° F. to about 2443° F., or about 2368° F. to about2855° F. for nickel; about 2358° F. to about 2458° F. or about 2373° F.to about 2423° F., or about 2358°to about 2805° F. for cobalt; about1932° F. to about 2032° F., about 1957° F. to about 2007° F., or about1932° F. to about 2467° F. for a copper/gold/silver alloy; about 399° F.to about 499° F., about 424° F. to about 474° F., or about 399° F. toabout 932° F. for a tin/lead/zinc alloy; about 399° F. to about 499° F.,about 424° F. to about 474° F., or about 399° F. to 932° F. for atin/sodium/potassium/magnesium alloy; about 2550° F. to about 2650° F.,about 2575° F. to about 2625° F., or about 2550° F. to about 2905° F.for silicon; about 2058° F. to about 2158° F., about 2073° F. to about2123° F., or about 2058° F. to about 2855° F. for iron; about 2058° F.to about 2158° F., about 2073° F. to about 2123° F., or about 2058° F.to about 2855° F. for an iron/vanadium/chromium/manganese alloy; or2368° F. to about 2468° F., about 2393° F. to about 2443° F., or about2368° F. to about 2855° F. for a nickel/tantalum/hafnium/tungsten alloy.

Inert gas or gases can be added during a step. Inert gases are chosen,independently, from the group consisting of argon, nitrogen, helium,neon, xenon, krypton, hydrogen, and mixtures thereof. When an inert gasis added during a step, the inert gas (or mixture thereof) can changefrom cycle-to-cycle or within a cycle.

For purposes of the present invention, inert gases used for purging,particularly in the backspace of a reactor are generally consideredseparately from the other inert gases. Nitrogen is typically addedcontinuously through a method of the present invention, irrespective ofwhether “inert gas” flow into the metal is started or stopped. In oneexample, a nitrogen flow is maintained throughout an entire method, suchthat a nitrogen pressure of about 0.4-0.6 psi, or about 0.5 psi ismaintained.

At the end of the instant methods, the molten metal or alloy is cooled.The metal or alloy is cooled, at minimum, to a temperature below thesolidus temperature. Preferably, the metal or alloy is cooled to room orambient temperature. Such cooling can include gradual and/or rapidcooling steps. Gradual cooling typically includes cooling due to heatexchange with air or an inert gas over 1 to 72 hours, 2 to 50 hours, 3to 30 hours, or 8 to 72 hours. Rapid cooling, also known as quenching,typically includes an initial cooling with air or an inert gas to belowthe solidus temperature, thereby forming a solid mass, and placing thesolid mass into a bath comprising a suitable fluid such as tap water,distilled water, deionized water, other forms of water, inert gases (asdefined above), liquid nitrogen or other suitable liquified gases, athermally-stable oil (e.g., silicone oil) or organic coolant, andcombinations thereof. The bath should contain a suitable quantity ofliquid at a suitable temperature, such that the desired amount ofcooling occurs.

Methods of the present invention are carried out in a suitable reactor.Suitable reactors are selected depending on the amount of metal or alloyto be processed, mode of heating, extent of heating (temperature)required, and the like. A preferred reactor in the present method is aninduction furnace reactor, which is capable of operating in a frequencyrange of 0 kHz to about 10,000 kHz, 0 kHz to about 3,000 kHz, or 0 kHzto about 1,000 kHz. Reactors operating at lower frequencies aredesirable for larger metal charges, such that a reactor operating at0-3,000 kHz is generally suitable for 20 pound metal charges and areactor operating at 0-1,000 kHz is generally suitable for 5000 poundmetal charges.

Typically, reactors of the present method are lined with a suitablecrucible. Crucibles are selected, in part, based on the amount of metalor alloy to be heated and the temperature of the method. Cruciblesselected for the present method typically have a capacity from aboutfive pounds to about five tons. One preferred crucible is comprised of89.07% Al₂O₃, 10.37% SiO₂, 0.16% TiO₂, 0.15% Fe₂O₃, 0.03% CaO, 0.01%MgO, 0.02% Na₂O₃, and 0.02% K₂O, and has a 9″ outside diameter, a 7.75″inside diameter, and a 14″ depth. A second preferred crucible iscomprised of 99.68% Al₂O₃, 0.07% SiO₂, 0.08% Fe₂O₃, 0.04% CaO, and 0.12%Na₂O₃, and has a 4.5″ outside diameter, a 3.75″ inside diameter and a10″ depth.

After being subjected to a process of the present invention, metals andalloys can be analyzed by a variety of techniques, including chemicaland physical methods. A preferred analytical method is x-rayfluorescence spectrometry. X-ray fluorescence spectrometry is describedin “X-Ray Fluorescence Spectrometry”, by George J. Havrilla in “Handbookof Instrumental Techniques for Analytical Chemistry,” Frank A. Settle,Ed., Prentice-Hall, Inc: 1997, which is incorporated herein byreference.

XRF spectrometry is a well-known and long-practiced method, which hasbeen used to detect and quantify or semi-quantify the elementalcomposition (for elements with Z≧11) of solid and liquid samples. Thistechnique benefits from minimal sample preparation, wide dynamic range,and being nondestructive. Typically, XRF data are not dependent on whichdimension (e.g., axial or radial) of a sample was analyzed. Accuracy ofless than 1% error can generally be achieved with XRF spectrometry, andthe technique can have detection limits of parts per million.

XRF spectrometry first involves exciting an atom, such that an innershell electron is ejected (e.g., the photoelectric effect). Uponejection of an electron, an outer shell electron will “drop” down intothe lower-energy position of the ejected inner shell electron. When theouter shell electron “drops” into the lower-energy inner shell, x-rayenergy is released. Typically, an electron is ejected from the K, L, orM shell and is replaced by an electron from the L, M, or N shell.Because there are numerous combinations of ejections and replacementspossible for any given element, x-rays of several energies are emittedduring a typical XRF experiment. Therefore, each element in the PeriodicTable has a standard pattern of x-ray emissions after being excited by asufficiently energetic source, since each such element has its owncharacteristic electronic state. By matching a pattern of emitted x-rayenergies to values found in tables, such as those on pages 10-233 to10-271 of “Handbook of Chemistry and Physics, 73^(rd) Edition,” editedby D. R. Lide, CRC Press, 1992, which is incorporated herein byreference, one can identify which elements are present in a sample. Inaddition, the intensity of the emitted x-rays allows one to quantify theamount of an element in a sample.

There are two standard variations of the XRF technique. First, as anenergy-dispersive method (EDXRF), the XRF technique uses a detector suchas a Si(Li) detector, which is capable of simultaneously measuring theenergy and intensity of x-ray photons from an array of elements. EDXRFis well-suited for rapid acquisition of data to determine grosselemental composition. Typically, the detection limits for EDXRF are inthe range of tens to hundreds of parts-per-million. Awavelength-dispersive technique (WDXRF) is generally better-suited foranalyses requiring high accuracy and precision. WDXRF uses a crystal todisperse emitted x-rays, based on Bragg's Law. Natural crystals, such aslithium fluoride and germanium, are commonly used for high-energy (shortwavelength) x-rays, while synthetic crystals are commonly used forlow-energy (longer wavelength) x-rays. Crystals are chosen, in part, toachieve desired resolution, so that x-rays of different energies aredisperse to distinguishable 2θ angles. WDXRF can either measure x-rayssequentially, such that a WDXRF instrument will step through a range of2θ angles in recording a spectrum, or there will be detectors positionedat multiple 2θ angles, allowing for more rapid analysis of a sample.Detectors for WDXRF commonly include gas ionization and scintillationdetectors. A further description of the use WDXRF technique in thepresent invention can be found in Example 1. Results from EDXRF andresults from WDXRF can be compared by determining the relationshipbetween a 2θ angle and the wavelength of the corresponding x-ray (e.g.,using Bragg's Law) and converting the wavelength into an energy (e.g.,energy equals wavelength multiplied by Planck's constant).

Analysis of emitted x-rays can be carried out automatically orsemi-automatically, such as by using a software package (e.g., UniQuant,which is sold by Omega Data Systems BV, Veldhoven, The Netherlands) foreither EDXRF or WDXRF. UniQuant is used for standardlesssemi-quantitative to quantitative XRF analysis using the intensitiesmeasured by a sequential x-ray spectrometer. The software packageunifies all types of samples into one analytical program. The UniQuantsoftware program is highly effective for analyzing samples for which nostandards are available. Sample preparation is usually minimal or notrequired at all. Samples can be of very different natures, sizes andshapes. Elements from fluorine or sodium up to uranium, or their oxidecompounds, can be analyzed in samples such as a piece of glass, a screw,metal drillings, lubricating oil, loose fly ash powder, polymers,phosphoric acid, thin layers on a substrate, soil, paint, the year ringsof trees, and, in general, those samples for which no standards areavailable. The reporting is in weight % along with an estimated errorfor each element.

In software packages such as UniQuant, an XRF spectrum is composed ofdata channels. Each data channel corresponds to an energy range andcontains information about the number of x-rays emitted at that energy.The data channels can be combined into one coherent plot to show thenumber or intensity of emitted x-rays versus energy or 2θ angle (the 2θangle is related to the wavelength of an x-ray), such that the plot willshow a series of peaks. An analysis of the peaks by one skilled in theart or the software package can identify the correspondence between theexperimentally-determined peaks and the previously-determined peaks ofindividual elements. For an element, peak location (i.e., the centroidof the peak with respect to energy or 2θ angle), peak profile/shape,peak creation, and peak fluidity would be expected to be essentially thesame, within experimental error, for any sample containing the element.If the same quantity of an element is present in two samples, intensitywill also be essentially the same, excepting experimental error andmatrix effects.

A typical software package is programmed to correlate certain datachannels with the emitted x-rays of elements. Quantification of theintensity of emitted x-rays is accomplished by integrating the XRFspectrum over a number of data channels. Based on the measuredintensities and the previously-compiled data on elements, the softwarepackage will integrate over all data channels, correlate the emittedx-ray intensities, and will then calculate the relative abundance orquantity of elements which appear to be present in a sample, based uponcomparison to the standards. Ideally, the relative abundances will total100% prior to normalization. However, for a variety of reasons, such asimproper or insufficient calibration, the relative abundances will nottotal 100% prior to normalization. Another reason that the relativeabundances of elements do not total 100% prior to normalization is thata portion of the XRF spectrum falls outside of the data channels thatthe software package correlates with an element (i.e., a portion of theXRF spectrum is not recognized as belonging to an element and is notincluded in the relative abundance calculation). In this case, therelative abundances will likely total less than 100% prior tonormalization. Representative examples of relative abundance data arepresented in Table 4, which includes the results of XRF analyses of theproducts of Examples 1-10, as processed by a Uniquant software package.

X-ray emission spectrometry (XES), a technique analogous to XRF, alsoprovides electronic information about elements. In XES, a lower-energysource is used to eject electrons from a sample, such that only thesurface (to several micrometers) of the sample is analyzed. Similar toXRF, a series of peaks is generated, which corresponds to outer shellelectrons replacing ejected inner shell electrons. The peak shape, peakfluidity, peak creation, peak intensity, peak centroid, and peak profileare expected to be essentially the same, within experimental error andmatrix effects, for two samples having the same composition.

A new composition of matter of the present invention can manifest itselfas a transient, adjustable, or permanent change in energy and/orassociated properties, as broadly defined. Property change can beexhibited as or comprise a change in: (1) structural atomic character(e.g., XES/XRF peak creation, peak fluidity, peak intensity, peakcentroid, peak profile or shape as a function of material/sampleorientation, atomic energy level(s), and TEM, STM, MFM scans); (2)electronic character (e.g., electron electromagnetic interactions,electromagnetic field position/orientation, energy gradients, Halleffect, voltage, capacitance, voltage decay rate, voltage gradient,voltage signature including slope of decay and/or change of slope decay,voltage magnitude, voltage orientation); (3) structural molecular oratomic character (e.g, SEM, TEM, STM, AFM, LFM, and MFM scans, opticalmicroscopy images, and structural orientation, ordering, long rangealignment/ordering, anisotropy); (4) physical constants (e.g., color,crystalline form, specific rotation, emissivity, melting point, boilingpoint, density, refractive index, solubility, hardness, surface tension,dielectric, magnetic susceptibility, coefficient of friction, x-raywavelengths); (5) physical properties (e.g., mechanical, chemical,electrical, thermal, engineering, and the like); and, (6) other changesthat differentiate naturally occurring materials from manufacturedmaterials created by inducing a change in matter.

1. Structural Atomic Character

In the sections below, certain analyses have been conducted where ablock of a manufactured product (e.g., a metal or an alloy) has been cutfrom a larger piece. In these analyses, the axial direction or an axialtrace refers to a side of the block that was originally parallel to theside walls of a reactor. The radial direction or a radial trace refersto a side of the block that was originally parallel with the top orbottom of a reactor. A metal block can also contain micro- ormacro-voids that can be analyzed. FIG. 1A shows a non-contact, magneticforce microscopy image of natural copper, the control standard, and FIG.1B shows a new composition of matter: manufactured copper, which isidentified by an altered and aligned electromagnetic network. FIG. 2Ashows a non-contact, magnetic force microscopy (MFM) scan and FIG. 2Bshows a scanning tunneling microscopy (STM) scan. Individually, and fromdiffering vantage points, these scans show the outline of the changedelectromagnetic energy network. The MFM scan shows the radial tracewhile the STM scan shows the axial trace.

XES analysis of the control standard compared to the atomically altered(i.e., manufactured) state are shown in FIGS. 3A, 3B, 4A, and 4B.Manufactured copper in the axial direction exhibits similar compositionto natural copper (i.e., 99.98%_(wt)), but radial scans exhibit newpeaks in the region close to naturally occurring S, Cl, and K. Theshifting centroid of the observed peaks from the natural species (i.e.,S, Cl, K) confirm electronic change in the atomic state of the baseelement; as does the non-contact MFM void scan (compare FIG. 1B withFIG. 5A). Conventional chemical analysis performed using a LECO (IR)analyzer confirmed the absence of sulfur at XES lower detection limits.LECO analysis confirmed sulfur concentration at 7.8 ppm; this analysiswas consistent with the manufacture's batch product analysis of 7.0 ppmS.

FIG. 5B compares the XES radial scan of manufactured copper to that of avoid space within the same material. An underlying change in atomiccharacter can be inferred from a dramatic change in signalcount/intensity and a non-contact MFM of the void space (FIG. 5A). MFMevidence highlights the structure and its changed orientation andalignment compared to the control MFM (FIG. 1A).

High precision XRF imaging shows that manufactured copper has a K_(α)line in the vicinity of 110.7 degrees (the 2θ angle). Since 110.7degrees is the location of natural sulfur's K_(α) line, this K_(α) lineis referred to herein as a “sulfur-like” K_(α) line. This is the K_(α)line that would be expected if detectable quantities of sulfur werepresent; however, an IR LECO analysis of this sample showed that therewas no sulfur was present (<10 ppm) in the sample. The presence of thisline indicates an electronic structure change, which has shifted the twotheta degree position of the K_(α) line compared to natural copper(FIGS. 6A and 6B). Several other figures indicate the presence ofunexpected K_(α) lines for elements not present in the sample (e.g.,FIG. 27 shows the presence of a significant aluminum-like K_(α) line fora sample containing 99.98% copper). FIG. 7 shows an increase in signalintensity dependent upon which side of a homogeneous block of sample wasanalyzed, as well as a shifting K_(α) centroid. These data demonstratemicroscopically the bulk anisotropy later identified in the manufacturedsample as does the MFM scans (FIGS. 1B and 5A).

2. Electronic Character

Manipulation of the electrodynamic components affecting the orientationof a manufactured metal's or alloy's electromagnetic field can enablethe observance of a Hall voltage (V_(H)). Manipulation of theelectrodynamic components enables intensification of electromagneticfield affording charge concentration on the surface of the atoms withinthe bulk as opposed to the bulk surface of the bath. Properties thatreflect field repositioning can include changing capacitance and voltagedecay rate (FIG. 8) and voltage gradients (FIG. 9) within a conductingbulk media.

FIG. 10 shows the V_(H) observed in a copper-nickel alloy. Voltage decayexhibited two distinct decay rates, indicative of two controllingmechanisms. A positive voltage signature with a positive capacitancedecay (i.e., capacitance accumulation) is shown in FIG. 11.

Control and manipulation of the charge signature (e.g., V_(H) profile,capacitance slope, voltage slope) provides evidence of the alteration,and manipulation of the underlying electronic state. FIG. 12 shows apositive voltage signature and a positive capacitance decay.Additionally, the voltage decay profile has changed: one profile has anegative slope while the other has a neutral slope. Further change inthe electronic structure enables the slope of the second voltage decayprofile to become positive (FIG. 13); note also the change in slope ofcapacitance decay. The metal system shown in FIG. 14 has an electronicstructure change that result in a nearly neutral decay in voltage andcapacitance. Measurements were repeated four times. FIG. 15 shows thatthe voltage can actually become negative, indicating that theorientation can also be manipulated. FIG. 16 shows the phenomena can beobserved under pressure. Table 1 is an XRF analysis using a Uniquantsoftware package that shows a multiplicity of energetically contiguousX-ray atomic energy levels. One energetically contiguous series isrepresented by Sm, Eu, Gd, Tb; the other is represented by P, S, So(i.e., sulfur as an oxide), Cl, and Ar. Table 2 is an XRF analysis usinga Uniquant software package that shows an energetically contiguousseries as Al, Si, P, S, So (i.e., sulfur as an oxide), Cl, Ar, K, andCa. Table 3 represents an experiment that utilized the same startingmaterial as Tables 1 and 2, however, the reported amount or abundance ofcopper after processing differs from the other tables. The differingrelative abundances of elements observed in Tables 1-3 are believed tocorrespond to the unexpected peaks seen in many of the XRF plots.

3. Structural Molecular/Atomic Character

New compositions of matter can be electronically modified to induce longrange ordering/alignment. In one new composition of matter, long rangeordering was induced in oxygen-free high conductivity (OFHC) copper.Optical microscopy and SEM imaging of the material verifies the degreeand extent of long range ordering achieved (FIGS. 17A, 17B, 17C, 18A,18B, and 18C). Under similar electronic conditions, long range orderingwas induced in high purity (99.99 %_(wt)) nickel. FIGS. 19A, 19B, 20A,and 20B show the optical microscopy imaging of the manufactured nickelmaterial. A comparison of alignment is shown in-run, at two differentpoints during processing, which highlights the adjustability of thealtered electronic state of the manufactured nickel.

Extensive atomic force microscopy and non-contact MFM imaging ofelectronically altered OFHC copper shows views of structuralconfigurations from a different perspective (FIGS. 21A, 21B, 21C, 22A,22B, and 22C). Non-contact MFM imaging shows clear pattern repetitionand intensity of the manufactured copper when compared to the naturalcopper. The manufactured copper represents a new composition of matterderived from natural copper, and the manufactured copper exhibitsanisotropic behavior.

4. Physical Constants

In one sequence of new compositions of matter, color changes in OFHCcopper were induced. The variation in color over four (4) new mattercompositions ranged from black (two intensities) to copper (2intensities) to gold (one intensity) to silver (one intensity). Whilenot being bound by theory, the alteration of copper's electronic statealong the continuum enables the new composition of matter's color to beadjusted along the continuum.

In another sequence of new compositions of matter, changes in thehardness of OFHC copper were induced. The variation in diamond pyramidhardness between different manufactured copper samples ranged from about25 to 90 (or 3 to 9 times higher than natural copper). Hardness changewas anisotropic.

In another new composition of matter, magnetism was induced in a highpurity, non-magnetic metal copper (e.g., 99.98 %_(wt)) in its elementalform (FIGS. 23A and 23B).

5. Physical Properties

In one sequence of new compositions of matter, ductility changes wereinduced in a high purity, ductile copper (99.98%_(wt)) in its elementalform. The variation in the engineering physical property of ductilityranged from brittle to semi-ductile to ductile to extremely ductile overfour (4) new matter compositions.

In one new composition of matter, the electrical reactance was increasedapproximately 3% above that of natural copper over the frequency rangeof 0 Hz to 100 kHz. In another new composition of matter, electricalsusceptance was increased approximately 20% above 99.98%_(wt) copper ofthe same chemical composition (i.e., the copper in its natural state).In another new composition of matter, electrical susceptance wasdecreased approximately 25% below 99.98%_(wt) copper of the samechemical composition (i.e., the copper in its natural state). Electricalsusceptance for these new matter compositions compared to the controlstandard (the material in its natural state) is shown in FIG. 24.

6. Additional Differentiations

In one sequence of new compositions of matter, which all used the sameraw materials, consumables, utilities, and materials of construction,the sum of element concentrations identified by XRF analysis variedconsiderably. Variations in elemental abundance determined by XRFUniquant prior to normalization over three (3) new matter compositionswere 99.5 %_(wt) (Table 3), 96.0 %_(wt) (Table 2), and 90.6 %_(wt)(Table 1). The apparent loss of matter between the recognized elementalstructures and the manufactured elemental structures differentiatesnaturally occurring materials from materials with modified electronicstructures (i.e., a new composition of matter).

While not being bound by theory, Applicant believes the conservation ofenergy requires that all mass, independent of magnitude and/orconfiguration, character, and/or dimension can be characterized by theallowed set of mathematical poles (defined as the operation zurn) andfurther characterized by the set of mathematical poles coalesced(defined as the isozurn value). An adjustment or manipulation of thezurn invokes a change in the isozurn value to a value different than itsnaturally occurring value, and accounts for the contribution of its reststate value, thereby modifying the electronic structure that defines thenatural state. A change in the isozurn value to a value different thanthat which specifies the natural state denotes a change in theunderlying electronic state of the specified species.

A change in the isozurn value is typically noted at the subatomic,atomic, or molecular level. While not being bound by theory, thecomplexity of energy interactions is believed to often impede singlevariable isolation. In these cases, a change in the electronic state ofthe specified species typically manifests itself as a change in aproperty value(s) from the naturally occurring state (e.g., theunaltered entropic driven ground state). Typical changes denoting achange in property value, which depart from the property valuespecifying its naturally occurring state, dictate a change in theisozurn value of that state.

Definitions of Acronyms

-   AO—Atomic Orbital-   SEM—Scanning electron microscopy-   TEM—Tunneling Electron Microscopy-   STM—Scanning Tunneling Microscopy-   AFM—Atomic Force Microscopy-   LFM—Lateral Force Microscopy-   MFM—Magnetic Force Microscopy-   XES—X-ray Emission Spectrometry-   XRF—X-ray Fluorescence Spectrometry

EXEMPLIFICATION Example 1

Experimental Procedure for Copper Run 14-01-01

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor (Inductotherm) fitted with a 75-30RPowertrak power supply was charged with 2500 g copper (99.98% purity)through its charging port. The reactor was fitted with a graphite capand a ceramic liner (i.e., the crucible, from Engineering Ceramics).During the entire procedure, a slight positive pressure of nitrogen(˜0.5 psi) was maintained in the reactor using a continuous backspacepurge. The reactor was heated to the metal charge liquidus point plus300° F., at a rate no greater than 300° F./hour, as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 kHz to 3000 kHz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN300temperature controller. Upon reaching 2300° F., the reactor was chargedwith an additional 2143 g copper over an hour.

The temperature was again increased to 2462° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the copper charge throughports located in the top plate. The copper was held at 2462° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thecopper became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2480° F. over 7 minutes. Thetemperature was then varied between 2480° F. and 2530° F. for 15 cycles.Each cycle consisted of raising the temperature continuously over 7minutes and lowering the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of thecopper was varied over another 5 cycles between 2480° F. and 2530° F.

After the fifth cycle, the reactor temperature was lowered to 2462° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the copper and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2459° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2459° F. and 2453° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2450° F. over 5 minutes. Thetemperature was varied between 2450° F. and 2441° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2438° F. over 5 minutes. Thetemperature was varied between 2438° F. and 2406° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2406° F. and 2419° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was cooled by lowering the induction furnacepower to 1 kW or less as the ingot cooled. The copper was then cooled toapproximately ambient temperature in water.

Analytical Protocols

X-ray Fluorescence

An ARL 8410 XRF was used to analyze each of the sample ingots. An ARL8410 is a sequential wavelength dispersive spectrometer (WDS). Specificemission lines are used to determine the presence or absence, and theconcentrations of various elements. Each characteristic x-ray line ismeasured in sequence by the instrument by controlling the instrumentgeometry.

FIG. 62 shows the general configuration of the ARL 8410 spectrometer.The WDS spectrometer relies on the fundamentals of x-ray diffraction,when x-ray fluorescence occurs when matter is bombarded by a stream ofhigh-energy incident x-ray photons. When the incident X-radiationstrikes the sample, the incident x-rays may be absorbed, scattered, ortransmitted for the measurement of the fluorescent yield.

The ARL 8410 utilizes an end-window rhodium (Rh) x-ray tube. Theend-window is composed of Be, and holds the tube at high vacuum. Thefilaments are heated giving off electrons by thermoionic emission. Thisbeam of electrons then bombards the target Rh anode across a 10-70 keVvoltage potential. Thus, primary x-rays are produced during thecollision. The emitted x-ray spectrum consists of (1) “Continuum” or“Bremstrahlung” radiation, (2) Characteristic x-ray lines of the targetmaterial (e.g., K and L series), and (3) Characteristic lines from anycontaminants. Thus, the primary spectrum appears as a series of sharpintense peaks arrayed over a broad hump of continuum radiation. The ARLis equipped with and uses two types of photon detectors, the FlowProportional Counter (FPC) and the Scintillation Counter (SC).

The manufactured metal samples are prepared by cutting a cube shape(approximately 1.1875″) from the center of the cooled ingot. An axialedge and a radial edge are then denoted. To provide a smooth surface foranalysis, the axial and radial faces are sequentially polished. Thesample faces are sanded to 400 grit, then a polishing wheel is employedwith 600 grit paper. Finally, a ≦1 μm polishing compound completes thesmoothing process. The sample is then cleaned with iso-propyl alcoholand placed in a sample cassette/holder. The sample holder is then loadedinto the XRF.

The orientation of the detector crystal with respect to the sample andthe photon detector is controlled synchronously such that characteristicx-ray lines can be accurately measured. A sequential measurementconsists of positioning the diffraction crystal at a given theta(diffraction angle) and the detector at two-theta and counting for agiven period of time. The crystal and detector are then rotated to adifferent angle for the next characteristic x-ray line.

Uniquant Version 2 software, developed by Omega Data Systems is used tocontrol the crystal and detector placement and provides the datareduction algorithms for each analytical protocol. The sample resultsinclude an elemental composition list along with the associatedconcentrations for each sample.

Measurement of Grain Sizes

When the grain sizes exceeded the size discernible with the human eye,the grain size (average span distance) was measured using a micrometer.When the grain sizes were not discernible via the naked eye, standardacid etching was performed and then optical microscopy was utilized tomeasure and characterize the grain.

Measurement of Magnetism

The magnetic properties of the manufactured ingots were tested via threemethods.

-   Magnetic Attraction: An ⅛″ diameter neodymium iron boron magnet was    scanned consistently and uniformly across the surface of the ingot    to detect areas of attraction. Areas of attraction were then noted    at specific sites on the surface.-   Attraction to Iron: The attraction of iron filings to specific    points on the ingot were quantified by enumerating the number of    filings retained on the ingot surface in a vertical or upside-down    orientation.-   Gauss Measurement: The magnetic behavior of various points on the    ingot were quantified via the use of a F. W. Bell 4048 Gauss meter.    Measurement of Chemical Reactivity

The manufactured ingots were subjected to various chlorine ligands,including NaCl, NaOCl, HCl, and chlorinated organics tosemi-quantitatively access their reactivity to ligated chlorine. Theformation of reaction products was recorded, then reaction products wereremoved from the reaction site, weighed and elemental compositionverified via XRF.

Analytical Results

An x-ray fluorescence analysis of the copper sample is provided in FIG.26, with the K_(α) peak of a copper control standard shown forreference.

An x-ray fluorescence analysis of the copper sample is provided in FIG.27, with the K_(α) peak of an aluminum control standard shown forreference.

Summary data showing the apparent elemental composition of the productof Example 1 is shown in Tables 5-13, as was measured by an XRF analysisusing a Uniquant software package. The apparent elemental composition ofthe product varies by position, which is indicated in each table.

The manufactured copper exhibited large grain sizes and differentcoloration on each grain, which caused the surface to appear iridescent.The axial (top) face of the ingot appeared glassy, while the sides weremetallic in appearance (due to anisotropic behavior). The color on boththe axial and radial surfaces mimicked that of natural copper (i.e., notthe intense reds or dark browns observed in other manufactured coppers,for example, Examples 11-14). On the axial surface, unique demarcationswere observed. The ingot had some internal void areas, which were opento the top surface. No unexpected magnetic activity or chemicalreactivity were recorded.

Example 2

Experimental Procedure for Nickel Run 14-01-04

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm, was fittedwith a 75-30R Powertrak power supply and charged with 2500 g nickel(99.97% purity) and 100 g of graphite carbon through its charging port.The reactor was fitted with a graphite cap with a ceramic liner (i.e.the crucible, from Engineering Ceramics). During the entire procedure, aslight positive pressure of nitrogen (˜0.5 psi) was maintained in thereactor using a continuous backspace purge. The reactor was heated tothe metal charge liquidus point, over a rate no greater than 300°F./hour, as limited by the integrity of the crucible. The inductionfurnace operated in a frequency range of 0 kHz to 3000 kHz, withfrequency determined by a temperature-controlled feedback loopimplementing an Omega Model CA 300 temperature controller. Upon reaching2800° F., the reactor was charged with an additional 2700 g nickel overan hour.

The temperature was again increased to 2850° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity [<5 ppm impurities]graphite rods) were inserted to the bottom of the nickel charge throughports located in the top plate. The nickel was held at 2850° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thenickel became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 3256° F. over 7 minutes. Thetemperature was then varied between 2950° F. and 3256° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered and a0.15 L/min flow of argon was begun. The temperature of the nickel wasvaried over another 5 cycles between 2950° F. and 3256° F.

After the fifth cycle, the reactor temperature was lowered to 2850° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the nickel and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2829° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2790° F. and 2829° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2770° F. over 5 minutes. Thetemperature was varied between 2710° F. and 2770° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2691° F. over 5 minutes. Thetemperature was varied between 2492° F. and 2691° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2571° F. and 2492° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature over 15 minutes. The gas additionlance was removed.

The reactor temperature was slowly cooled by lowering the inductionfurnace power to 1 KW or less as the ingot cooled. The nickel was thencooled to approximately ambient temperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the nickel sample is provided in FIGS.28A and 28B, with the K_(α) and L_(α) peaks of a nickel control standardshown for reference.

An x-ray fluorescence analysis of the nickel sample is provided in FIG.29A, with the K_(α) peak of an aluminum control standard shown forreference.

An x-ray fluorescence analysis of the nickel sample is provided in FIG.29B, with the K_(α) peak of a zirconium control standard shown forreference.

An x-ray fluorescence analysis of the nickel sample is provided in FIG.30A, with the K_(α) peak of a sulfur control standard shown forreference.

An x-ray fluorescence analysis of the copper sample is provided in FIG.30B, with the K_(α) peak of an chlorine (from potassium chloride) shownfor reference. Summary data showing the apparent elemental compositionof the product of Example 2 is shown in Tables 14-16, as was measured byan XRF analysis using a Uniquant software package. The apparentelemental composition of the product varies by position, which isindicated in each table.

The manufactured nickel retained a large amount of refractory on itsexterior surface after retrieval from the reactor. The retainedrefractory was attributed to either surface attraction or reaction withthe high content of Al₂O₃ in the refractory. The ingot did not crackwith handling, but did have an internal void. The visible radial surfaceappeared duller in than the axial (top) face, again demonstratinganisotropic physical properties. The ingot demonstrated no unexpectedchemical reactivity after removal from the reaction system.

Example 3

Experimental Procedure for Cobalt Run 14-01-05

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm and fitted witha 75-30R Powertrak power supply, was charged with 2176 g cobalt (99.8%purity) through its charging port. The reactor was fitted with agraphite cap with a ceramic liner from Engineering Ceramics. During theentire procedure, a slight positive pressure of nitrogen (˜0.5 psi) wasmaintained in the reactor using a continuous backspace purge. Thereactor was heated to 2800° F. over a minimum of 14 hours while theinduction furnace operated in a frequency range of 0 kHz to 3000 kHz.Upon reaching 2700° F., the reactor was charged with an additional 3000g cobalt over an hour.

When 2800° F. was reached, graphite saturation assemblies were insertedto the bottom of the cobalt charge through ports located in the topplate. The cobalt was held at 2800° F. for 4 hours. Every 30 minutesduring the hold period, an attempt was made to lower the graphitesaturation assemblies as dissolution progressed. As the cobalt becamesaturated with carbon, the graphite saturation assemblies were consumed.After the 4 hour hold period was complete, the graphite saturationassemblies were removed.

The reactor temperature was increased to 3086° F. over 7 minutes. Thetemperature was then varied between 2875° F. and 3086° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered and a0.15 L/min flow of argon was begun. The temperature of the cobalt wasvaried over another 5 cycles between 2875° F. and 3086° F. After thefifth cycle, the reactor temperature was lowered to 2800° F. over a 10minute period with continued argon addition. The graphite saturationassemblies were reinstalled in the cobalt and remained there for 1 hour.The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2785° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2689° F. and 2785° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2737° F. over 5 minutes. Thetemperature was varied between 2689° F. and 2737° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2672° F. over 5 minutes. Thetemperature was varied between 2498° F. and 2672° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2570° F. and 2498° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed. The reactor temperature was cooled bylowering the induction furnace power to 1 kW or less as the ingotcooled. The cobalt was then cooled to approximately ambient temperaturein water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the cobalt sample is provided in FIGS.31A and 31B, with the K_(α) and L_(α) peaks of a cobalt control standardshown for reference.

An x-ray fluorescence analysis of the cobalt sample is provided in FIG.32A, with the K_(α) peak of an aluminum control standard shown forreference.

An x-ray fluorescence analysis of the cobalt sample is provided in FIG.32B, with the K_(α) peak of an iron control standard shown forreference.

An x-ray fluorescence analysis of the cobalt sample is provided in FIG.33A, with the K_(α) peak of a chlorine (from potassium chloride) controlstandard shown for reference.

An x-ray fluorescence analysis of the cobalt sample is provided in FIG.33B, with the K_(α) peak of a zirconium control standard shown forreference.

An x-ray fluorescence analysis of the cobalt sample is provided in FIG.34, with the K_(α) peak of a manganese control standard shown forreference.

Summary data showing the apparent elemental composition of the productof Example 3 is shown in Table 17, as was measured by an XRF analysisusing a Uniquant software package.

The top (axial) face of the manufactured cobalt ingot exhibited many ofthe recursive patterns observed in other manufactured ingots. Thesurface peaks are inconsistent with what would be expected given theforces of gravity during cooling. In addition, the shiny top face of theingot exhibited an unexpected coloration, such that some of the faceshad a distinct pink tint. While the top of the ingot was shiny, silvermetallic, the sides of the ingot were matte silver in appearance.

The manufactured cobalt ingot retained a small amount of refractoryaround its base. The ingot did not crack upon retrieval from thereaction system. No unexpected magnetic behavior or chemical reactivitywere observed.

Example 4

Experimental Procedure for Copper/Gold/Silver Run 14-01-06

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm and fitted witha 75-30R Powertrak power supply was charged with 2518 g copper (99.98%purity), plus 62.28 g each of gold (99.9999% pure) and silver (99.9999%pure) through its charging port. The reactor was fitted with a graphitecap with a ceramic liner by Engineering Ceramics. During the entireprocedure, a slight positive pressure of nitrogen (˜0.5 psi) wasmaintained in the reactor using a continuous backspace purge. Thereactor was heated to 2300° F. over a minimum of 12 hours while theinduction furnace operated in a frequency range of 0 kHz to 3000 kHz.Upon reaching 2300° F., the reactor was charged with an additional 2000g copper over an hour.

The temperature was again increased to 2462° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies were inserted to the bottom of the metal chargethrough ports located in the top plate. The alloy was held at 2462° F.for 4 hours. Every 30 minutes during the hold period, an attempt wasmade to lower the graphite saturation assemblies. As the alloy becamesaturated with carbon, the graphite saturation assemblies were consumed.After the 4 hour hold period was complete, the graphite saturationassemblies were removed.

The reactor temperature was increased to 2480° F. over 7 minutes. Thetemperature was then varied between 2480° F. and 2530° F. for 15 cycles.Each cycle consisted of raising the temperature continuously over 7minutes and lowering the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered and a0.15 L/min flow of argon was begun. The temperature of the alloy wasvaried over another 5 cycles between 2480° F. and 2530° F.

After the fifth cycle, the reactor temperature was lowered to 2462° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the alloy and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2459° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2453° F. and 2459° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2450° F. over 5 minutes. Thetemperature was varied between 2441° F. and 2450° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2438° F. over 5 minutes. Thetemperature was varied between 2406° F. and 2438° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2406° F. and 2419° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed. The reactor temperature was cooled bylowering the induction furnace power to 1 kW or less as the ingotcooled. The copper/silver/gold was then cooled to approximately ambienttemperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the copper/gold/silver alloy sample isprovided in FIG. 35, with the K_(α) peak of a copper control standardshown for reference.

An x-ray fluorescence analysis of the copper/gold/silver alloy sample isprovided in FIG. 36, with the K_(α) peak of a gold control standardshown for reference.

An x-ray fluorescence analysis of the copper/gold/silver alloy sample isprovided in FIG. 37, with the K_(α) peak of a silver control standardshown for reference.

Summary data showing the apparent elemental composition of the productof Example 4 is shown in Tables 18-19, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The manufactured copper-based alloy exhibited uniform coloration in boththe axial and radial directions. Prior to being quenched in water, theingot exhibited significant iridescence on all surfaces. After beingquenched, the intensity of iridescence diminished.

An unexpected feature of the ingot was the axial face crystalorientation. No magnetic behavior was observed. The ingot did not crackor retain any refractory after retrieval from the reactor.

Example 5

Experimental Procedure for Tin/Lead/Zinc 14-01-07

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm and fitted witha 75-30R Powertrak power supply was charged with 2562 g copper (99.9%purity), plus 854 g each of Lead (99+% pure) and Zinc (99.8% pure)through its charging port. The reactor was fitted with a graphite capwith a ceramic liner by Engineering Ceramics. During the entireprocedure, a slight positive pressure of nitrogen (˜0.5 psi) wasmaintained in the reactor using a continuous backspace purge. Thereactor was heated to 932° F. over a minimum of 4 hours at a rate nogreater than 300° F./hour. The induction furnace operated in thefrequency range of 0 kHz to 3000 kHz with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN300temperature controller.

When 932° F. was reached, graphite saturation assemblies were insertedto the bottom of the metal charge through ports located in the topplate. The tin/lead/zinc alloy was held at 932° F. for 4 hours. Every 30minutes during the hold period, an attempt was made to lower thegraphite saturation assemblies. As the tin/lead/zinc alloy becamesaturated with carbon, the graphite saturation assemblies were consumed.After the 4 hour hold period was complete, the graphite saturationassemblies were removed.

The reactor temperature was increased to 968° F. over 7 minutes. Thetemperature was then varied between 942° F. and 968° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of thetin/lead/zinc alloy was varied over another 5 cycles between 942° F. and968° F.

After the fifth cycle, the reactor temperature was lowered to 932° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the tin/lead/zinc alloy andremained there for 1 hour. The graphite saturation assemblies wereremoved.

The reactor temperature was lowered to 930° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 918° F. and 930° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 924° F. over 5 minutes. Thetemperature was varied between 918° F. and 924° F. over 4½ cycles. Eachcycle consisted of lowering the temperature continuously over 5 minutesand raising the temperature continuously over 3 minutes. In addition,while raising the temperature, a 0.15 L/min flow of argon was added, andwhile lowering the temperature, a 0.15 L/min flow of nitrogen was added.

The reactor temperature was lowered to 916° F. over 5 minutes. Thetemperature was varied between 894° F. and 916° F. for 15.5 cycles. Eachcycle consisted of lowering the temperature continuously over 15 minutesand raising the temperature over 15 minutes. In addition, while raisingthe temperature, a 0.15 L/min flow of argon was added, and whilelowering the temperature, a 0.15 L/min flow of nitrogen was added. Allgas addition, except for the purge of nitrogen ceased after the 15.5cycles were completed.

The temperature was varied between 894° F. and 903° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed. The reactor temperature was cooled bylowering the induction furnace power to 1 kW or less as the ingotcooled. The tin/lead/zinc alloy was then cooled to approximately ambienttemperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the tin/lead/zinc alloy sample isprovided in FIG. 38, with the K_(α) peak of a tin control standard shownfor reference.

An x-ray fluorescence analysis of the tin/lead/zinc alloy sample isprovided in FIG. 39, with the K_(α) peak of a zinc control standardshown for reference.

An x-ray fluorescence analysis of the tin/lead/zinc alloy sample isprovided in FIG. 40, with the K_(α) peak of a lead control standardshown for reference.

Summary data showing the apparent elemental composition of the productof Example 5 is shown in Tables 20-21, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The manufactured tin-based alloy exhibited some stratification along thesides of the ingot. The top (axial) face and the side (radial) face didnot appear significantly different in coloration or appearance, and eachhad a matte finish. Like other manufactured alloy ingot, apparent peakswere exhibited on the axial face of the ingot.

The ingot did not have an internal void. No unexpected chemical activityor magnetic activity were recorded. The ingot did not crack uponretrieval from the reactor and retained a small amount of refractory.

Example 6

Experimental Procedure for Tin/Sodium, Magnesium and Potassium 14-01-08

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductothenm and fitted witha 75-30R Powertrak power supply, was charged with 2000 g tin (99.9%purity), plus 50 g each of sodium (99.8% pure), potassium (98% pure) andmagnesium (99.98% pure) through its charging port. The reactor wasfitted with a graphite cap with a ceramic liner (i.e. the crucible, fromEngineering Ceramics). During the entire procedure, a slight positivepressure of nitrogen (˜0.5 psi) was maintained in the reactor using acontinuous backspace purge. The reactor was heated to the metal chargeliquidus point plus 300° F., at a rate no greater than 300° F./hour, aslimited by the integrity of the crucible. The induction furnace operatedin the frequency range of 0 kHz to 3000 kHz, with frequency determinedby a temperature-controlled feedback loop implementing an Omega ModelCN300 temperature controller. Upon reaching 900° F., the reactor wascharged with an additional 2120 g Sn over an hour.

The temperature was again increased to 932° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the Sn/Na/K/Mg chargethrough ports located in the top plate. The Sn/Na/K/Mg alloy was held at932° F. for 4 hours. Every 30 minutes during the hold period, an attemptwas made to lower the graphite saturation assemblies as dissolutionoccurred. As the Sn/Na/K/Mg alloy became saturated with carbon, thegraphite saturation assemblies were consumed. After the 4 hour holdperiod was complete, the graphite saturation assemblies were removed.

The reactor temperature was increased to 968° F. over 7 minutes. Thetemperature was then varied between 942° F. and 968° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of theSn/Na/K/Mg alloy was varied over another 5 cycles between 942° F. and968° F.

After the fifth cycle, the reactor temperature was lowered to 932° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in thetin/sodium/potassium/magnesium alloy and remained there for 1 hour. Thegraphite saturation assemblies were removed.

The reactor temperature was lowered to 930° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 918° F. and 930° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 924° F. over 5 minutes. Thetemperature was varied between 918° F. and 924° F. over 4½ cycles. Eachcycle consisted of lowering the temperature continuously over 5 minutesand raising the temperature continuously over 3 minutes. In addition,while raising the temperature, a 0.15 L/min flow of argon was added, andwhile lowering the temperature, a 0.15 L/min flow of nitrogen was added.

The reactor temperature was lowered to 916° F. over 5 minutes. Thetemperature was varied between 894° F. and 916° F. for 15.5 cycles. Eachcycle consisted of lowering the temperature continuously over 15 minutesand raising the temperature continuously over 15 minutes. In addition,while raising the temperature, a 0.15 L/min flow of argon was added, andwhile lowering the temperature, a 0.15 L/min flow of nitrogen was added.All gas addition, except for the purge of nitrogen ceased after the 15.5cycles were completed.

The temperature was varied between 894° F. and 903° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed. The reactor temperature was cooled bylowering the induction furnace power to 1 kW or less as the ingotcooled. The tin/sodium/magnesium/potassium alloy solidified into aningot. After solidification, the alloy was cooled to approximatelyambient temperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the tin/sodium/potassium/magnesiumalloy sample is provided in FIG. 41, with the K_(α) peak of a potassium(from potassium chloride) control standard shown for reference.

An x-ray fluorescence analysis of the tin/sodium/potassium/magnesiumalloy sample is provided in FIG. 42, with the K_(α) peak of a tincontrol standard shown for reference.

An x-ray fluorescence analysis of the tin/sodium/potassium/magnesiumalloy sample is provided in FIG. 43, with the K_(α) peak of a magnesiumcontrol standard shown for reference.

An x-ray fluorescence analysis of the tin/sodium/potassium/magnesiumalloy sample is provided in FIG. 44, with the K_(α) peak of a sodium(from AlNa₃F₆) control standard shown for reference.

Summary data showing the apparent elemental composition of the productof Example 6 is shown in Tables 22-23, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The ingot had a uniform dull matte finish on axial and radial surfaces(i.e., isotropic coloration). Minimal refractory was retained uponretrieval from the reactor. No internal voids were found in the ingot.No unexpected magnetic or chemical activity were observed.

Example 7

Experimental Procedure for Silicon 15-01-01

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor (Inductotherm) fitted with a 75-30RPowertrak power supply was charged with 700 g Silicon (100.00% purity),through its charging port. The reactor was fitted with a graphite capand a ceramic liner (i.e., the crucible, from Engineering Ceramics).During the entire procedure, a slight positive pressure of nitrogen(˜0.5 psi) was maintained in the reactor using a continuous backspacepurge. The reactor was heated to the metal charge liquidus point plus300° F., at a rate no greater than 300° F./hour as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 kHZ to 3000 kHz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN 300temperature controller. Upon reaching 2800° F., the reactor was chargedwith an additional 400 g Silicon again using a rate no greater than 300°F./hour.

The temperature was again increased to 2900° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (5 ppm impurities)graphite rods) were inserted to the bottom of the Silicon charge throughports located in the top plate. The Silicon was held at 2900° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As theSilicon became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2976° F. over 7 minutes. Thetemperature was then varied between 2920° F. and 2976° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of theSilicon was varied over another 5 cycles between 2920° F. and 2976° F.

After the fifth cycle, the reactor temperature was lowered to 2900° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the Silicon and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2895° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2886° F. and 2895° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2873° F. over 5 minutes. Thetemperature was varied between 2868° F. and 2873° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2863° F. over 5 minutes. Thetemperature was varied between 2811° F. and 2863° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2833° F. and 2811° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was slowly cooled by lowering the inductionfurnace power to 1 kW or less s the ingot cooled. After solidification,the Silicon was cooled to approximately ambient temperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the silicon sample is provided inFIGS. 45A and 45B, with the K_(α) and L_(α) peaks of a silicon controlstandard shown for reference.

An x-ray fluorescence analysis of the silicon sample is provided in FIG.46A, with the K_(α) peak of an aluminum control standard shown forreference.

An x-ray fluorescence analysis of the silicon sample is provided in FIG.46B, with the K_(α) peak of a titanium control standard shown forreference.

An x-ray fluorescence analysis of the silicon sample is provided in FIG.47A, with the K_(α) peak of a sulfur control standard shown forreference.

An x-ray fluorescence analysis of the silicon sample is provided in FIG.47B, with the K_(α) peak of a chlorine (from potassium chloride) controlstandard shown for reference.

An x-ray fluorescence analysis of the silicon sample is provided in FIG.48A, with the K_(α) peak of a gallium control standard shown forreference.

An x-ray fluorescence analysis of the silicon sample is provided in FIG.48B, with the K_(α) peak of a potassium control standard shown forreference.

Summary data showing the apparent elemental composition of the productof Example 7 is shown in Tables 24-27, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

No unexpected magnetic activity or chemical reactivity were recorded forthe ingot. The manufactured silicon system did appear shiny on its axial(top) face and dull on is radial (side) face. The ingot retained minimalrefractory upon removal from the reactor.

Example 8

Experimental Procedure for Iron 15-01-02

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm, fitted with a75-30R Powertrak power supply was charged with 2000 g Iron (99.98%purity) and 200 g carbon through its charging port. The reactor wasfitted with a graphite cap with a ceramic liner (i.e. the crucible, fromEngineering Ceramics). During the entire procedure, a slight positivepressure of nitrogen (˜0.5 psi) was maintained in the reactor using acontinuous backspace purge. The reactor was heated to the metal chargeliquidus point plus 300° F., at a rate no greater than 300° F./hour, aslimited by the integrity of the crucible. The induction furnace operatedin the frequency range of 0 kHz to 3000 kHz, with frequency determinedby a temperature-controlled feedback loop implementing an Omega ModelCN300 temperature controller. Upon reaching 2800° F., the reactor wascharged with an additional 2595 g iron over an hour.

The temperature was again increased to 2850° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the iron charge throughports located in the top plate. The iron was held at 2850° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As theiron became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 3360° F. over 7 minutes. Thetemperature was then varied between 2993° F. and 3360° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of theiron was varied over another 5 cycles between 2993° F. and 3360° F.

After the fifth cycle, the reactor temperature was lowered to 2850° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the iron and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2819° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2622° F. and 2818° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2724° F. over 5 minutes. Thetemperature was varied between 2622° F. and 2724° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2586° F. over 5 minutes. Thetemperature was varied between 2133° F. and 2586° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2340° F. and 2133° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was cooled by lowering the induction furnacepower to 1 kW or less as the ingot cooled. After solidification, theiron was cooled to approximately ambient temperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the iron sample is provided in FIGS.49A and 49B, with the K_(α) and L_(α) peaks of an iron control standardshown for reference.

An x-ray fluorescence analysis of the iron sample is provided in FIG.50A, with the K_(α) peak of an aluminum control standard shown forreference.

An x-ray fluorescence analysis of the iron sample is provided in FIG.50B, with the K_(α) peak of an zirconium control standard shown forreference.

An x-ray fluorescence analysis of the iron sample is provided in FIG.51A, with the K_(α) peak of a sulfur control standard shown forreference.

An x-ray fluorescence analysis of the iron sample is provided in FIG.51B, with the K_(α) peak of a chlorine (from potassium chloride) controlstandard shown for reference.

Summary data showing the apparent elemental composition of the productof Example 8 is shown in Tables 28-29, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The manufactured iron exhibited no unexpected magnetic activity. Thereactivity relative to that which would be expected from natural ironhas not been quantified. The ingot appears glassy or shiny on its axial(top) face and dull on its radial (side) face. The manufactured ironretained a negligible amount of refractory upon removal from thereactor, but cracked upon retrieval. The ingot had no internal voids.

Example 9

Experimental Procedure for Iron W/Vanadium, Chromium and Manganese15-01-03

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm, fitted with a75-30R Powertrak power supply, was charged with 2000 g Iron (99.98%purity), plus 91.9 g each of Vanadium (99.5% pure), Chromium (99% pure),and Manganese (99.9% pure), plus 200 g of carbon through its chargingport. The reactor was fitted with a graphite cap with a ceramic liner(i.e., the crucible, from Engineering Ceramics). During the entireprocedure, a slight positive pressure of nitrogen (˜0.5 psi) wasmaintained in the reactor using a continuous backspace purge. Thereactor was heated to the metal charge liquidus point plus 300° F., at arate no greater than 300° F./hour as limited by the integrity of thecrucible. The induction furnace operated in the frequency range of 0 kHzto 3000 kHz, with frequency determined by a temperature-controlledfeedback loop implementing an Omega Model CN300 temperature controller.Upon reaching 2800° F., the reactor was charged with an additional2319.3 g iron over an hour.

The temperature was again increased to 2850° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity graphite rods) wereinserted to the bottom of the metal charge through ports located in thetop plate. The alloy was held at 2850° F. for 4 hours. Every 30 minutesduring the hold period, an attempt was made to lower the graphitesaturation assemblies as dissolution occurred. As the alloy becamesaturated with carbon, the graphite saturation assemblies were consumed.After the 4 hour hold period was complete, the graphite saturationassemblies were removed.

The reactor temperature was increased to 3360° F. over 7 minutes. Thetemperature was then varied between 2993° F. and 3360° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of theiron was varied over another 5 cycles between 2993° F. and 3360° F.

After the fifth cycle, the reactor temperature was lowered to 2850° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the iron and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2819° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2622° F. and 2818° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2724° F. over 5 minutes. Thetemperature was varied between 2622° F. and 2724° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2586° F. over 5 minutes. Thetemperature was varied between 2133° F. and 2586° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2340° F. and 2133° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was cooled by lowering the induction furnacepower to 1 kW or less as the ingot cooled. Theiron/vanadium/chromium/manganese alloy was the cooled to approximatelyambient temperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the iron/vanadium/chromium/manganesealloy sample is provided in FIG. 52, with the K_(α) peak of a chromium(from chromium(III) oxide) control standard shown for reference.

An x-ray fluorescence analysis of the iron/vanadium/chromium/manganesealloy sample is provided in FIG. 53, with the K_(α) peak of an ironcontrol standard shown for reference.

An x-ray fluorescence analysis of the iron/vanadium/chromium/manganesealloy sample is provided in FIG. 54, with the K_(α) peak of a vanadiumcontrol standard shown for reference.

An x-ray fluorescence analysis of the iron/vanadium/chromium/manganesealloy sample is provided in FIG. 55, with the K_(α) peak of a manganesecontrol standard shown for reference.

An x-ray fluorescence analysis of the iron/vanadium/chromium/manganesealloy sample is provided in FIG. 56, in the region of the K_(α) peak ofa sulfur control standard.

Summary data showing the apparent elemental composition of the productof Example 9 is shown in Tables 40-41, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

Upon polishing the manufactured alloy in preparation for XRF analysis,the alloy was noted to be particularly hard and a stratification patternthat was not attributable to the polishing materials was exposed. Therelative hardness of the alloy was tested and the Moh's hardness wasfound to be greater than what would be expected from a natural alloy ofa similar composition. The radial surface of the ingot had a shiny orglassy appearance, while the axial surface appeared dull, thusreflecting bulk anisotropic behavior.

The manufactured alloy had no unexpected magnetic activity. The ingotretained a negligible amount of refractory upon retrieval from thereactor, but did crack.

Example 10

Experimental Procedure for Nickel W/Tantalum, Hafnium and Tungsten15-01-04

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5″ O.D.×3.75″ I.D.×10″ depth) of a 100pound induction furnace reactor supplied by Inductotherm, fitted with a75-30R Powertrak power supply and was charged with 2500 g Nickel (99.9%purity), plus 100 g each of Hafnium (99.9% pure), W (99.9% pure), Ta(99.98% pure), and carbon through its charging port. The reactor wasfitted with a graphite cap with a ceramic liner (i.e., the crucible,from Engineering Ceramics). During the entire procedure, a slightpositive pressure of nitrogen (˜0.5 psi) was maintained in the reactorusing a continuous backspace purge. The reactor was heated to the metalcharge liquidus point plus 300° F., at a rate no greater than 300°F./hour, as limited by the integrity of the crucible. The inductionfurnace operated in the frequency range of 0 kHz to 3000 kHz, withfrequency determined by a temperature-controlled feedback loopimplementing an Omega Model CN300 temperature controller. Upon reaching2800° F., the reactor was charged with an additional 2200 g nickel overan hour.

The temperature was again increased to 2850° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the metal charge throughports located in the top plate. The alloy was held at 2850° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thealloy became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 3256° F. over 7 minutes. Thetemperature was then varied between 2950° F. and 3256° F. for 15 cycles.Each cycle consisted of lowering the temperature continuously over 7minutes and raising the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 0.15 L/min flow of argon was begun. The temperature of thealloy was varied over another 5 cycles between 2950° F. and 3256° F.

After the fifth cycle, the reactor temperature was lowered to 2850° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the alloy and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2829° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2790° F. and 2829° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2770° F. over 5 minutes. Thetemperature was varied between 2710° F. and 2770° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2691° F. over 5 minutes. Thetemperature was varied between 2492° F. and 2691° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of argon wasadded, and while lowering the temperature, a 0.15 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2571° F. and 2492° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was slowly cooled by lowering the inductionfurnace power to 1 kW or less as the ingot cooled. After solidification,the alloy was cooled to approximately ambient temperature in water.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

An x-ray fluorescence analysis of the nickel/hafnium/tantalum/tungstenalloy sample is provided in FIG. 57, with the K_(α) peak of a tantalumcontrol standard shown for reference.

An x-ray fluorescence analysis of the nickel/hafnium/tantalum/tungstenalloy sample is provided in FIG. 58, with the K_(α) peak of a tungstencontrol standard shown for reference.

An x-ray fluorescence analysis of the nickel/hafnium/tantalum/tungstenalloy sample is provided in FIG. 59, with the K_(α) peak of a hafniumcontrol standard shown for reference.

An x-ray fluorescence analysis of the nickel/hafnium/tantalum/tungstenalloy sample is provided in FIG. 60, in the region of the K_(α) peak ofa sulfur control standard.

An x-ray fluorescence analysis of the nickel/hafnium/tantalum/tungstenalloy sample is provided in FIG. 61, with the K_(α) peak of a nickelcontrol standard shown for reference.

Summary data showing the apparent elemental composition of the productof Example 10 is shown in Tables 30-31, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The manufactured nickel-based alloy exhibited clear anisotropic behaviorwith respect to color and reactivity similar to the anisotropy observedvia XRF. The sides were covered with a large amount of refractoryretained after the ingot was retrieved from the reactor. The top facehad a classic metallic sheen. No unexpected magnetic activity wasobserved. The ingot did not upon removal from the reactor or exhibit anyinternal voids.

Example 11

Experimental Procedure for Copper 14-00-01

A cylindrical alumina-based crucible (89.07% Al₂O₃, 10.37% SiO₂, 0.16%TiO₂, 0.15% Fe₂O₃, 0.03% CaO, 0.01% MgO, 0.02% Na₂O₃, 0.02% K₂O; 9″O.D.×7.75″ I.D.×14″ depth) of a 100 pound induction furnace reactorsupplied by Inductotherm, fitted with a 75-30R Powertrak power supply,was charged with 100 pounds copper (99.98% purity) through its chargingport. During the entire procedure, a slight positive pressure ofnitrogen (˜0.5 psi) was maintained in the reactor using a continuousbackspace purge. The reactor was heated to the metal charge liquiduspoint plus 300° F., at a rate no greater than 300° F./hour, as limitedby the integrity of the crucible. The induction furnace operated in thefrequence range of 0 kHz to 3000 kHz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN300temperature controller.

The temperature was again increased to 2462° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the copper charge throughports located in the top plate. The copper was held at 2462° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thecopper became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2480° F. over 7 minutes. Thetemperature was then varied between 2480° F. and 2530° F. for 15 cycles.Each cycle consisted of raising the temperature continuously over 7minutes and lowering the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 1.5 L/min flow of argon was begun. The temperature of thecopper was varied over another 5 cycles between 2480° F. and 2530° F.

After the fifth cycle, the reactor temperature was lowered to 2462° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the copper and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2459° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2459° F. and 2453° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2450° F. over 5 minutes. Thetemperature was varied between 2450° F. and 2441° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2438° F. over 5 minutes. Thetemperature was varied between 2438° F. and 2406° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2406° F. and 2419° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was rapidly cooled by quenching in water, sothat the copper solidified into an ingot.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

Summary data showing the apparent elemental composition of the productof Example 11 is shown in Tables 32-33, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

Immediately after the method described above was completed, multiplediscrete magnetic spots attracted by a ⅛″ diameter neodymium iron boronmagnet were observed in a sinusoidal pattern. The ingot exhibited pointattraction to iron filings at reduced temperatures at or near 77 K. Overdays to months, the strength of the magnetic attraction decreased on afraction of the locations exhibiting magnetic attraction or attractionto iron filings.

Various forms of ligated chlorine (e.g., HCl and MCl, where M is a metalas defined above) readily reacted with the manufactured copper formyielding product distributions distinguishable from natural copper,thereby demonstrating a change in chemical reactivity. This reactivityincreased over time.

Extremely large grain sizes (i.e., greater than 1″) were observed, whichis uncharacteristic and previously unreported in natural copper systems(typically, copper grains sizes are 10-100 μm). Unique changes incoloration were observed with the crossing of grain boundaries; however,the overall coloration mimicked natural copper.

Example 12

Experimental Procedure for Copper 14-00-03

A cylindrical alumina-based crucible (89.07% Al₂O₃, 10.37% SiO₂, 0.16%TiO₂, 0.15% Fe₂O₃, 0.03% CaO, 0.01% MgO, 0.02% Na₂O₃, 0.02% K₂O; 9″O.D.×7.75″ I.D.×14″ depth) of a 100 pound induction firnace reactorsupplied by Inductotherm, fitted with a 75-30R Powertrak power supplyand was charged with 100 pounds copper (99.98% purity) through itscharging port. During the entire procedure, a slight positive pressureof nitrogen (˜0.5 psi) was maintained in the reactor using a continuousbackspace purge. The reactor was heated to the metal charge liquiduspoint plus 300° F., at a rate no greater than 300° F./hour, as limitedby the integrity of the crucible. The induction furnace operated in thefrequence range of 0 kHz to 3000 kHz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN300temperature controller.

The temperature was again increased to 2462° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the copper charge throughports located in the top plate. The copper was held at 2462° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thecopper became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2480° F. over 7 minutes. Thetemperature was then varied between 2480° F. and 2530° F. for 15 cycles.Each cycle consisted of raising the temperature continuously over 7minutes and lowering the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 1.5 L/min flow of argon was begun. The temperature of thecopper was varied over another 5 cycles between 2480° F. and 2530° F.

After the fifth cycle, the reactor temperature was lowered to 2462° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the copper and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2459° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2459° F. and 2453° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2450° F. over 5 minutes. Thetemperature was varied between 2450° F. and 2441° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2438° F. over 5 minutes. Thetemperature was varied between 2438° F. and 2406° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2406° F. and 2419° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was rapidly cooled by quenching in water, sothat the copper solidified into an ingot.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

Summary data showing the apparent elemental composition of the productof Example 12 is shown in Tables 34-35, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

This manufactured copper system demonstrated an ability to change color(i.e., visible light spectrum emission) dependent upon electromagneticstimulation. The color of the top, glassy surface of an ingot changedunder different lighting conditions. While the (radial) side of theingot was a matte pink color, the top of the ingot (axial face) has aglassy color, which can vary from intense burgundy to golden bronze toburnished orange. These differences in appearance reflect the anisotropydetected via the XRFs.

The radial surface of the ingot was covered with magnetically activespots. The magnetism of the ingot decreased over time. Altered chemicalreactivity, particularly with respect to ligated chlorine, was observedon axial surfaces. The chemical reactivity increased over time. Radialsurfaces appeared unaffected and were free from refractory (materialfrom the crucible).

Example 13

Experimental Procedure for Copper 14-00-04

A cylindrical alumina-based crucible (89.07% Al₂O₃, 10.37% SiO₂, 0.16%TiO₂, 0.15% Fe₂O₃, 0.03% CaO, 0.01% MgO, 0.02% Na₂O₃, 0.02% K₂O; 9″O.D.×7.75″ I.D.×14″ depth) of a 100 pound induction furnace reactorsupplied by Inductotherm, fitted with a 75-30R Powertrak power supplywas charged with 100 pounds copper (99.98% purity) through its chargingport. During the entire procedure, a slight positive pressure ofnitrogen (˜0.5 psi) was maintained in the reactor using a continuousbackspace purge. The reactor was heated to the metal charge liquiduspoint plus 300° F., at a rate no greater than 300° F./hour, as limitedby the integrity of the crucible. The induction furnace operated in thefrequence range of 0 kHz to 3000 kHz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN300temperature controller.

The temperature was again increased to 2462° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the copper charge throughports located in the top plate. The copper was held at 2462° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thecopper became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2480° F. over 7 minutes. Thetemperature was then varied between 2480° F. and 2530° F. for 15 cycles.Each cycle consisted of raising the temperature continuously over 7minutes and lowering the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 1.5 L/min flow of argon was begun. The temperature of thecopper was varied over another 5 cycles between 2480° F. and 2530° F.

After the fifth cycle, the reactor temperature was lowered to 2462° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the copper and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2459° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2459° F. and 2453° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2450° F. over 5 minutes. Thetemperature was varied between 2450° F. and 2441° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2438° F. over 5 minutes. Thetemperature was varied between 2438° F. and 2406° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2406° F. and 2419° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was slowly cooled and was subsequently quenchedin water, so that the copper solidified into an ingot.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

Summary data showing the apparent elemental composition of the productof Example 13 is shown in Tables 36-37, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The manufactured copper ingot exhibited many of the characteristicpatterns observed in previous examples. Differences in the colorationand appearance of the axial and radial directions were observed: matte,burgundy brown coloration on the side, and glassy on the top withdemarcations.

This ingot had internal voids. The ingot demonstrated enhanced chemicalreactivity on the axial surfaces. Refractory was found to be tightlybound to select portions of the radial surfaces. Minimal magneticactivity was detected.

Example 14

Experimental Procedure for Copper 15-00-01

A cylindrical alumina-based crucible (89.07% Al₂O₃, 10.37% SiO₂, 0.16%TiO₂, 0.15% Fe₂O₃, 0.03% CaO, 0.01% MgO, 0.02% Na₂O₃, 0.02% K₂O; 9″O.D.×7.75″ I.D.×14″ depth) of a 100 pound induction furnace reactorsupplied by Inductotherm, fitted with a 75-30R Powertrak power supplyand was charged with 100 pounds copper (99.98% purity) through itscharging port. During the entire procedure, a slight positive pressureof nitrogen (˜0.5 psi) was maintained in the reactor using a continuousbackspace purge. The reactor was heated to the metal charge liquiduspoint plus 300° F., at a rate no greater than 300° F./hour, as limitedby the integrity of the crucible. The induction furnace operated in thefrequence range of 0 kHz to 3000 kHz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN300temperature controller.

The temperature was again increased to 2462° F. again using a rate nogreater than 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜″ OD, 36″ long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the copper charge throughports located in the top plate. The copper was held at 2462° F. for 4hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thecopper became saturated with carbon, the graphite saturation assemblieswere consumed. After the 4 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2480° F. over 7 minutes. Thetemperature was then varied between 2480° F. and 2530° F. for 15 cycles.Each cycle consisted of raising the temperature continuously over 7minutes and lowering the temperature continuously over 7 minutes. Afterthe 15 cycles were completed, a gas addition lance was lowered into themolten metal to a position approximately 2″ from the bottom of thereactor and a 1.5 L/min flow of argon was begun. The temperature of thecopper was varied over another 5 cycles between 2480° F. and 2530° F.

After the fifth cycle, the reactor temperature was lowered to 2462° F.over a 10 minute period with continued argon addition. The graphitesaturation assemblies were reinstalled in the copper and remained therefor 1 hour. The graphite saturation assemblies were removed.

The reactor temperature was lowered to 2459° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued argonaddition. The temperature was then varied between 2459° F. and 2453° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. The argon addition ceased after completion of the 20cycles.

The reactor temperature was lowered to 2450° F. over 5 minutes. Thetemperature was varied between 2450° F. and 2441° F. over 4½ cycles.Each cycle consisted of lowering the temperature continuously over 5minutes and raising the temperature continuously over 3 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added.

The reactor temperature was lowered to 2438° F. over 5 minutes. Thetemperature was varied between 2438° F. and 2406° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 1.5 L/min flow of argon wasadded, and while lowering the temperature, a 1.5 L/min flow of nitrogenwas added. All gas addition, except for the purge of nitrogen ceasedafter the 15.5 cycles were completed.

The temperature was varied between 2406° F. and 2419° F. for one cycle.The cycle consisted of raising the temperature continuously over 15minutes and lowering the temperature continuously over 15 minutes. Thegas addition lance was removed.

The reactor temperature was slowly cooled and was subsequently quenchedin water, so that the copper solidified into an ingot.

Analytical Protocols

XRF, grain size, magnetism, and chemical reactivity measurements werecarried out by the procedures described in Example 1.

Analytical Results

Summary data showing the apparent elemental composition of the productof Example 14 is shown in Tables 38-39, as was measured by an XRFanalysis using a Uniquant software package. The apparent elementalcomposition of the product varies by position, which is indicated ineach table.

The manufactured copper demonstrated an ability to change color (i.e.,visible light spectrum emission), dependant upon electromagneticstimulation. The top (axial face) of the ingot can vary from intenseburgundy to a deep golden orange. Additionally, the appearance and colorof this ingot reflect the anisotropy detected via the XRF scans. Theradial (side) face appears like burnished copper, while the axial (top)face has a glassy appearance.

On the bottom and side faces, each of the grain boundaries is clearlydelineated. Each of the grains appears to have a different color, givingthe exterior of the ingot an iridescent appears. The ingot did not havean internal void, as ingots of previous examples did. Additionally, theingot did not exhibit the extensive magnetic activity observed inExamples 11 and 12. The ingot retained an extensive amount of refractoryupon retrieval from the reactor.

While this invention has been particularly shown and described withreferences to preferred embodiments thereof, it will be understood bythose skilled in the art that various changes in form and details may bemade therein without departing from the scope of the inventionencompassed by the appended claims. TABLE 1 ANALYSIS REPORT by UniquantSpectrometers configuration: ARL 8410 Rh 60 kV LiF220 LiF420 Ge111 TlAPSample ident = Tailored - 3 Further info = Kappa list = 15-Nov-94Channel list = 23-Sep-99 Calculated as: Elements Spectral impurity data:CAL.209Teflon X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <10 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0 0.037 29 + Cu 99.58 0.03 51 Sb < 11 Na < 30 + Zn <2e 0.006 52 Te< 12 Mg < 31 + Ga 0.012 0.003 53 I < 13 + Al 0.027 0.012 32 Ge <2e 0.00355 Cs < 14 Si < 33 As < 56 Ba < 15 + P 0.003 0.001 34 Se < SumLa . . .Lu 0.15 0.07 16 + S 0.038 0.003 35 Br < 72 + Hf <2e 0.022 16 + So 0.0220.003 37 Rb < 73 + Ta <2e 0.071 17 + Cl 0.037 0.003 38 Sr < 74 W < 18 +Ar 0.017 0.002 39 Y < 75 Re < 19 + K <2e 0.0008 40 Zr < 76 Os < 20 + Ca0.0050 0.0008 41 Nb < 77 + Ir 0.029 0.008 21 Sc < 42 Mo < 78 + Pt 0.0170.007 22 + Ti 0.015 0.001 44 Ru < 79 Au <2e 0.007 23 V < 45 Rh < 80 Hg <24 Cr < 46 Pd < 81 Tl < 25 + Mn 0.0069 0.0007 47 Ag < 82 Pb < 26 + Fe0.015 0.001 48 + Cd 0.004 0.002 83 Bi < 27 Co < 49 In < 90 Th <2e 0.00328 Ni < 50 Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44Ru < 57 + La 0.073 0.006 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47Ag < 60 Nd < 8 O 75 Re < 62 + Sm 0.022 0.003 9 F < 76 Os < 63 + Eu 0.0150.002 77 + Ir 0.029 0.008 64 + Gd 0.009 0.002 78 + Pt 0.017 0.007 65 +Tb 0.015 0.002 79 Au <2e 0.007 66 Dy < 67 + Ho <2e 0.013 68 Er <2e 0.00469 Tm < 70 Yb <2e 0.005 71 + Lu <2e 0.013 KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 90.6%

TABLE 2 ANALYSIS REPORT by Uniquant Spectrometers configuration: ARL8410 Rh 60 kV LiF220 LiF420 Ge111 TlAP Sample ident = Tailored - 2Further info = Kappa list = 15-Nov-94 Channel list = 23-Sep-99Calculated as: Elements Spectral impurity data: CAL.209Teflon X-ray path= Vacuum Film type = No supporting film Case number = 0 Known Area, %Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mm Eff.Area = 490.6mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass = 18000.00 mgSample Height = 5 mm < means that the concentration is <10 ppm <2e meanswt % <2 StdErr. The + in Z + El means involved in Sum = 100% Z wt %StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.036 29 + Cu 98.620.06 51 Sb < 11 + Na 0.11 0.02 30 + Zn <2e 0.006 52 Te < 12 Mg < 31 + Ga0.007 0.003 53 I < 13 + Al 0.44 0.03 32 Ge <2e 0.003 55 Cs < 14 + Si0.107 0.008 33 As < 56 Ba < 15 + P 0.004 0.001 34 Se < SumLa . . . Lu0.087 0.072 16 + S 0.19 0.01 35 Br < 72 + Hf < 16 + So 0.12 0.01 37 Rb <73 + Ta <2e 0.071 17 + Cl 0.17 0.01 38 Sr < 74 W < 18 + Ar 0.027 0.00239 Y < 75 Re < 19 + K 0.0065 0.0010 40 Zr < 76 Os < 20 + Ca 0.013 0.00141 Nb < 77 Ir < 21 Sc < 42 Mo < 78 + Pt 0.022 0.008 22 + Ti 0.015 0.00144 Ru < 79 Au <2e 0.007 23 V < 45 Rh < 80 Hg < 24 Cr < 46 Pd < 81 Tl <25 Mn <2e 0.0006 47 Ag < 82 Pb < 26 + Fe 0.044 0.004 48 Cd <2e 0.002 83Bi < 27 Co < 49 In < 90 Th < 28 Ni < 50 Sn < 92 U < Light Elements NobleElements Lanthanides 4 Be 44 Ru < 57 + La 0.059 0.005 5 B 45 Rh < 58 Ce<2e 0.003 6 C 46 Pd < 59 Pr <2e 0.003 7 N 47 Ag < 60 Nd <2e 0.002 8 O 75Re < 62 Sm <2e 0.003 9 F < 76 Os < 63 Eu < 77 Ir < 64 Gd < 78 + Pt 0.0220.008 65 + Tb 0.005 0.002 79 Au <2e 0.007 66 Dy <2e 0.008 67 + Ho <2e0.015 68 Er <2e 0.004 69 Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0D/S = 0Sum Conc's before normalisation to 100%: 96.0%

TABLE 3 ANALYSIS REPORT by UniQuant Spectrometers configuration: ARL8410 Rh 60 kV LiF220 LiF420 Ge111 TlAP Sample ident = Tailored - 1Further info = Kappa list = 15-Nov-94 Channel list = 20-Jul-94Calculated as: Elements Spectral impurity data: CAL.209Teflon X-ray path= Vacuum Film type = No supporting film Case number = 0 Known Area, %Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mm Eff.Area = 490.6mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass = 18000.00 mgSample Height = 5 mm < means that the concentration is <10 ppm <2e meansthat Conc <2 × StdErr Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0 0.036 29 Cu 99.84 0.03 51 Sb < 11 Na < 30 Zn < 52 Te < 12 Mg <31 Ga 0.007 0.003 53 I < 13 Al < 32 Ge <2e 0.002 55 Cs < 14 Si < 33 As <56 Ba < 15 P < 34 Se < SumLa . . . Lu 0.053 0.071 16 S 0.0089 0.0008 35Br < 72 Hf <2e 0.022 16 So < 37 Rb < 73 Ta < 17 Cl 0.017 0.001 38 Sr <74 W < 18 Ar < 39 Y < 75 Re < 19 K <2e 0.0007 40 Zr < 76 Os < 20 Ca0.0024 0.0009 41 Nb < 77 Ir 0.040 0.008 21 Sc <2e 0.001 42 Mo 0.0050.002 78 Pt < 22 Ti 0.003 0.001 44 Ru < 79 Au <2e 0.006 23 V < 45 Rh <80 Hg <2e 0.006 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 Fe <48 Cd < 83 Bi < 27 Co < 49 In < 90 Th 0.009 0.003 28 Ni < 50 Sn < 92 U <Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La 0.030 0.0065 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re <62 Sm < 9 F < 76 Os < 63 Eu <2e 0.002 77 Ir 0.040 0.008 64 Gd <2e 0.00278 Pt < 65 Tb <2e 0.002 79 Au <2e 0.006 66 Dy < 67 Ho <2e 0.015 68 Er0.014 0.004 69 Tm <2e 0.004 70 Yb < 71 Lu <2e 0.014 KnownConc = 0 REST =0 D/S = 0Sum Conc's before normalisation to 100%: 99.5%

TABLE 4 XRF Analyses of Manufactured Ingots 14-00-01 Cu 14-00-03 Cu14-00-04 Cu 15-00-001 Cu 14-01-01 Cu Atom No. Element Axial Radial AxialRadial Axial Radial Axial Radial Axial Radial Major Elements: 11 Na0.063 0.11

0.29 0.07 0.062

0.048 0.058 12 Mg 13 Al 0.33 0.23 0.103 0.37 0.27 0.83 0.29 0.33 0.030.67 14 Si 0.55 0.58 0.018 0.29 0.29 0.6

0.89 0.51 19 K 0.021 0.013 0.0023

23 V 24 Cr 0.002 25 Mn 26 Fe 27 Co 28 Ni 29 Cu 95.55 95.34

95.93 99.29 98.59

95.07 95.09 30 Zn 47 Ag

0.004 50 Sn 72 Hf 73 To 74 W 79 Au 62 Pb Minor Elements 4-9 Be-F 0.110.071 15 P 0.004 16 S 0.0042 0.0065 0.0058 0.021 0.012 0.0043 0.0030 16So 0.0074 0.0057 0.0026 17 Cl 0.026 0.029 0.037 0.063 0.021 0.02 0.0210.034 0.0107 0.0065 18 Ar 0.013 0.015 0.018 0.013 0.012 0.016 0.0150.017 0.009 0.006 20 Ca 0.0041 0.0048 0.047 0.0109 0.0026 0.0078 21 Sc0.0038 0.0021 0.004 22 Ti 0.003 0.0037 31 Ga 0.008 0.003 0.005 0.0070.006 0.006 32

40 Zr 0.005 41 Nb 42 Mo 0.005 44

45 Rn 45 Co 51 Sb 56 Be 67-71 Lanthanides 0.021 0.011 0.0

0.005 0.023 0.021 0.014 0.012 0.003 0.014 75 R

77

0.018 0.031 0.023 0.029 0.035 0.038 0.031 0.026 90 Th Sum of Concen

100 99.6 99.4 90 99.5 88.1 89.7 94.6 101.7 102.1 Before Normol

14-01-04 Ni 15-01-01 Si 15-01-02 Fe 14-01-05 Co 14-01-06 Au/Ag Atom No.Element Axial Radial Axial Radial Axial Radial Axial Radial Axial RadialMajor Elements: 11 Na

0.12 0.004 0.013

0.026 0.043 0.066 0.045 12 Mg 13 Al

1.18 1.48

4.9 3.71

14 Si 0.03 0.14 98.88 98.12 0.032 0.14 0.073 0.10 19 K 0.0045 0.014

23 V 24 Cr 0.0031 0.0025 25 Mn 0.0091 0.0081 26 Fe 0.055 0.042

0.13 0.13 27 Co 94.6 95.7 28 Ni

0.0051 0.0053 0.16 0.18 29 Cu 0.012 0.0101 0.012 0.014 95.27 97.54 30 Zn0.0021 0.002 47 Ag 1.49

50 Sn 72 Hf 0.003 0.014 73 To 74 W 0.007 0.011

79 Au

62 Pb Minor Elements 4-9 Be-F 0.059 15 P 0.002 0.013 0.018 0.0023 0.00360.004 0.0037 16 S 0.013 0.0632 0.0066 16 So 0.0042 0.020 0.14 0.00770.012 17 Cl 0.005 0.004 0.019 0.014 0.0044 0.0047 0.0034 0.02 0.0

18 Ar 0.04 0.013 0.012 0.012 0.013 0.011 0.01 0.01

0.011 20 Ca 0.011 0.0092 0.077 0.0052 0.0073 0.0075 0.0067 0.0023 0.00821 Sc 0.0024 0.0025 0.0026 0.0022 0.0033 22 Ti 0.019 0.029 31 Ga 0.00360.0043 0.002 32

0.005 40 Zr 0.027 0.032 0.00

0.012 0.010 0.017 0.0034 0.005 41 Nb 42 Mo 44

45 Rn 0.003 45 Co 0.003 51 Sb 56 Be 0.005 0.005 0.006 67-71 Lanthanides0.

0.65 0.004 0.005 0.02 0.02 0.012 0.003 75 R

0.021 77

0.025 0.038 90 Th 0.006 Sum of Concen

104.4 100.5 63.4 79.7 9

97.5 102 101.3 100.1 1001 Before Normol

15-01-04 15-01-03 14-01-07 14-01-08 W/T a/Hf V/Cr/Mn/Fe Pb/Zn/SnSn/Na/K/Mg Atom No. Element Axial Radial Axial Radial Axial Radial AxialRadial Major Elements: 11 Na 0.056 0.043 0.032

1.67 2.02 12 Mg 0.013 0.018

13 Al 3.67 3.30 2.25

0.11 2.05

14 Si 0.23 0.74 0.13 0.026 0.010

19 K

23 V

24 Cr 2.71 2.39 25 Mn 2.05 2.2 26 Fe

27.9 0.017

27 Co 0.083 28 Ni 90.5 90

0.007 0.021

29 Cu 0.025 0.16 0.014 0.24 0.079 0.14 30 Zn 0.095 0.032 33.2 25.4 0.00347 Ag 50 Sn 47.9 54.7

72 Hf 1.78 2

73 To 1.76 1.78 74 W 1.49 1.5

0.033 0.031 0.048 79 Au 62 Pb 18.3 16.9

0.063 Minor Elements 4-9 Be-F 15 P 0.0025 0.0038 0.0097 0.0022 16 S0.0069 0.0053 16 So 0.0092 0.046 0.036 0.044 0.062 17 Cl 0.0044 0.00590.

0.092 0.031 0.053 0.015 0.0

18 Ar 0.018 0.019 0.009 0.01 20 Ca 0.0025 0.005 0.05 21 Sc 0.0036 0.002

22 Ti 0.003 31 Ga 32

40 Zr 0.043 0.092 0.016 0.024 0.027 0.043 41 Nb 42 Mo 44

0.011 45 Rn 45 Co 0.025 0.014 0.041 0.029 51 Sb 0.015 0.023 56 Be 67-71Lanthanides 0.58 0.57 0.031 0.035 0.021 0.025 75 R

77

90 Th 0.085 0.006 Sum of Concen

101 101.9 100.1 89.9 111.4 115.6 9

9

Before Normol

TABLE 5 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.347 of19-Jun-01 Today 19-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 AXIAL Further info =14-01-01 AXIAL 6/19 Kappa list = 15-Nov-94 Channel list = 18-Jun-01Calculated as: Elements Spectral impurity data: CAL.909 Teflon (7/94)X-ray path = Vacuum Film type = No supporting film Case number = 0 KnownArea, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mm Eff.Area= 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass =18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.03429 + Cu 98.07 0.07 51 Sb < 11 + Na 0.046 0.009 30 + Zn < 52 Te < 12 Mg <31 + Ga 0.006 0.003 53 I < 13 + Al 0.93 0.04 32 Ge < 55 Cs < 14 + Si0.89 0.04 33 As < 56 Ba <2e 0.003 15 + P < 34 Se < SumLa . . . Lu 0.0030.058 16 S 35 Br < 72 + Hf < 16 + So 0.0087 0.0008 37 Rb < 73 + Ta <17 + Cl 0.0107 0.0010 38 Sr < 74 W < 18 + Ar 0.009 0.002 39 Y < 75 Re <19 K < 40 Zr < 76 Os < 20 + Ca 0.0078 0.0008 41 Nb < 77 + Ir 0.025 0.00821 Sc < 42 Mo < 78 Pt <2e 0.007 22 Ti < 44 Ru < 79 Au < 23 V < 45 Rh <2e0.002 80 Hg <2e 0.006 24 Cr < 46 Pd < 81 Tl < 25 Mn 47 Ag <2e 0.002 82Pb <2e 0.003 26 Fe < 48 Cd < 83 Bi < 27 Co < 49 In < 90 Th <2e 0.003 28Ni < 50 Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru< 57 La < 5 B 45 Rh <2e 0.002 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e0.002 60 Nd < 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu <2e 0.001 77 + Ir0.025 0.008 64 Gd < 78 Pt <2e 0.007 65 Tb < 79 Au < 66 Dy < 67 Ho < 68Er < 69 Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 101.7%

TABLE 6 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.346 of19-Jun-01 Today 19-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 RADIAL Further info =14-01-01 RADIAL 6/19 Kappa list = 15-Nov-94 Channel list = 18-Jun-01Calculated as: Elements Spectral impurity data: CAL.909 Teflon (7/94)X-ray path = Vacuum Film type = No supporting film Case number = 0 KnownArea, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mm Eff.Area= 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass =18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0.071 0.03629 + Cu 98.69 0.06 51 Sb < 11 + Na 0.068 0.009 30 + Zn < 52 Te < 12 Mg <31 + Ga 0.006 0.003 53 I < 13 + Al 0.67 0.03 32 Ge < 55 Cs < 14 + Si0.51 0.03 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu 0.014 0.062 16S 35 Br < 72 + Hf < 16 + So 0.0026 0.0004 37 Rb < 73 + Ta < 17 + Cl0.0065 0.0009 38 Sr < 74 W < 18 + Ar 0.006 0.001 39 Y < 75 Re < 19 K <40 Zr < 76 Os < 20 Ca < 41 Nb < 77 + Ir <2e 0.008 21 + Sc 0.0040 0.000742 + 0.005 0.002 78 Pt < Mo 22 Ti < 44 Ru <2e 0.002 79 Au <2e 0.007 23 V< 45 Rh < 80 Hg < 24 + Cr < 46 Pd < 81 Tl < 25 Mn < 47 + Ag 0.004 0.00282 Pb < 26 Fe < 48 Cd < 83 Bi < 27 + Co < 49 In < 90 Th <2e 0.003 28 Ni< 50 Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru<2e 0.002 57 La < 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 + Ag0.004 0.002 60 Nd < 8 O 75 Re < 62 Sm < 9 F <2e 0.036 76 Os < 63 Eu <77 + Ir <2e 0.008 64 Gd < 78 Pt < 65 Tb < 79 Au <2e 0.007 66 Dy < 67 Ho< 68 + Er 0.012 0.003 69 Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0D/S = 0Sum Conc's before normalisation to 100%: 102.1%

TABLE 7 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.236 of23-Apr-01 Today 23-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 Cu SECTION TOP Furtherinfo = 14-01-01 MIDDLE SECTION TOP FACE AXIAL Kappa list = 15-Nov-94Channel list = 19-Apr-01 Calculated as: Elements Spectral impurity data:CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = No supporting filmCase number = 0 Known Area, % Rest, Diluent/Sample and Mass/AreaEff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0%Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm < meansthat the concentration is <20 ppm <2e means wt % <2 StdErr. The + in Z +El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt %StdErr SumBe . . . F 0 0.037 29 + Cu 99.71 0.03 51 Sb < 11 + Na 0.0980.011 30 + Zn < 52 Te < 12 Mg <2e 0.004 31 Ga <2e 0.003 53 I < 13 + Al0.066 0.005 32 Ge < 55 + Cs 0.007 0.003 14 Si < 33 As < 56 Ba < 15 + P <34 Se < SumLa . . . Lu 0.024 0.074 16 + S 0.014 0.001 35 Br < 72 + Hf <16 So 37 Rb < 73 + Ta < 17 + Cl 0.028 0.002 38 Sr < 74 W < 18 + Ar 0.0190.002 39 Y < 75 Re < 19 + K 0.0021 0.0007 40 Zr < 76 Os < 20 + Ca < 41Nb < 77 + Ir 0.024 0.008 21 Sc < 42 Mo < 78 Pt < 22 + Ti 0.0021 0.000944 Ru < 79 Au < 23 V < 45 Rh < 80 Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn <47 Ag < 82 Pb < 26 Fe < 48 + Cd 0.004 0.002 83 Bi < 27 Co < 49 In < 90 +Th 0.007 0.003 28 Ni < 50 Sn < 92 U < Light Elements Noble ElementsLanthanides 4 Be 44 Ru < 57 + La 0.015 0.004 5 B 45 Rh < 58 Ce < 6 C 46Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu< 77 + Ir 0.024 0.008 64 Gd <2e 0.002 78 Pt < 65 Tb < 79 Au < 66 Dy < 67Ho < 68 Er <2e 0.004 69 Tm <2e 0.005 70 Yb < 71 + Lu < KnownConc = 0REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 102.7%

TABLE 8 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.244 of19-Apr-01 Today 24-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 MID BOTTOM FACE Furtherinfo = 14-01-01 MIDDLE SECTION BOTTOM FCE AXIAL Kappa list = 15-Nov-94Channel list = 19-Apr-01 Calculated as: Elements Spectral impurity data:CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = No supporting filmCase number = 0 Known Area, % Rest, Diluent/Sample and Mass/AreaEff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0%Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm < meansthat the concentration is <20 ppm <2e means wt % <2 StdErr. The + in Z +El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt %StdErr SumBe . . . F 0 0.037 29 + Cu 98.42 0.06 51 Sb < 11 + Na 0.210.01 30 + Zn < 52 Te < 12 + Mg 0.013 0.004 31 + Ga 0.006 0.003 53 I <13 + Al 0.80 0.04 32 Ge < 55 Cs < 14 + Si 0.34 0.02 33 As < 56 Ba <2e0.003 15 + P < 34 Se < SumLa . . . Lu 0.018 0.071 16 + S 0.031 0.003 35Br < 72 + Hf <2e 0.022 16 So 37 Rb < 73 + Ta < 17 + Cl 0.070 0.006 38 +Sr 0.0024 0.0010 74 W < 18 + Ar 0.019 0.002 39 Y < 75 Re < 19 + K 0.0200.002 40 Zr < 76 Os <2e 0.006 20 + Ca 0.012 0.001 41 Nb < 77 + Ir 0.0330.008 21 Sc < 42 + Mo <2e 0.002 78 Pt < 22 + Ti 0.003 0.001 44 Ru < 79Au <2e 0.006 23 V < 45 Rh <2e 0.002 80 Hg <2e 0.006 24 Cr < 46 Pd < 81Tl < 25 Mn < 47 Ag < 82 + Pb 0.009 0.003 26 Fe <2e 0.001 48 + Cd 0.0040.002 83 Bi < 27 + Co < 49 In < 90 Th < 28 Ni < 50 Sn < 92 U < LightElements Noble Elements Lanthanides 4 Be 44 Ru < 57 La <2e 0.005 5 B 45Rh <2e 0.002 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re <62 Sm < 9 F < 76 Os <2e 0.006 63 Eu <2e 0.002 77 + Ir 0.033 0.008 64 Gd< 78 Pt < 65 Tb < 79 Au <2e 0.006 66 Dy < 67 Ho < 68 + Er 0.013 0.004 69Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 103.1%

TABLE 9 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.252 of19-Apr-01 Today 25-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 MID SECT TOP FACFurther info = 14-01-01 MIDDLE SECTION TOP FACE Apr. 25, 2001 Kappa list= 15-Nov-94 Channel list = 19-Apr-01 Calculated as: Elements Spectralimpurity data: CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = Nosupporting film Case number = 0 Known Area, % Rest, Diluent/Sample andMass/Area Eff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest= 0% Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm <means that the concentration is <20 ppm <2e means wt % <2 StdErr. The +in Z + El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt% StdErr SumBe . . . F 0 0.038 29 + Cu 99.66 0.03 51 Sb < 11 + Na 0.0340.011 30 + Zn < 52 Te < 12 Mg < 31 Ga <2e 0.003 53 I < 13 + Al 0.15 0.0132 Ge < 55 Cs < 14 + Si 0.033 0.005 33 As <2e 0.004 56 Ba <2e 0.003 15 +P < 34 Se < SumLa . . . Lu 0.026 0.075 16 + S 0.017 0.002 35 Br < 72 +Hf < 16 So 37 Rb < 73 + Ta < 17 + Cl 0.027 0.002 38 + Sr 0.003 0.001 74W < 18 + Ar 0.017 0.002 39 Y < 75 Re < 19 + K 0.0021 0.0007 40 Zr < 76Os <2e 0.007 20 + Ca 0.0056 0.0007 41 Nb < 77 + Ir 0.026 0.008 21 Sc <42 Mo < 78 Pt < 22 + Ti 0.0023 0.0010 44 Ru < 79 Au < 23 V < 45 Rh < 80Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 Fe < 48 Cd < 83Bi <2e 0.005 27 Co < 49 In < 90 Th <2e 0.003 28 Ni < 50 Sn < 92 U <Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 + La 0.0210.004 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75Re < 62 Sm < 9 F < 76 Os <2e 0.007 63 Eu < 77 + Ir 0.026 0.008 64 Gd <78 Pt < 65 Tb < 79 Au < 66 Dy < 67 Ho < 68 Er < 69 Tm <2e 0.005 70 Yb <71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 102.6%

TABLE 10 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.255 of19-Apr-01 Today 25-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 MID SECT TOP FACFurther info = 14-01-01 MIDDLE SECTION TOP FACE Apr. 25, 2001 Kappa list= 15-Nov-94 Channel list = 19-Apr-01 Calculated as: Elements Spectralimpurity data: CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = Nosupporting film Case number = 0 Known Area, % Rest, Diluent/Sample andMass/Area Eff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest= 0% Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm <means that the concentration is <20 ppm <2e means wt % <2 StdErr. The +in Z + El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt% StdErr SumBe . . . F 0 0.035 29 + Cu 99.70 0.03 51 Sb < 11 + Na <2e0.011 30 + Zn < 52 Te < 12 Mg < 31 Ga <2e 0.003 53 I < 13 + Al 0.14 0.0132 Ge < 55 Cs < 14 + Si 0.028 0.006 33 As < 56 Ba < 15 + P < 34 Se <SumLa . . . Lu 0.019 0.075 16 + S 0.018 0.002 35 Br < 72 + Hf < 16 So 37Rb < 73 + Ta < 17 + Cl 0.028 0.002 38 Sr < 74 W < 18 + Ar 0.020 0.002 39Y < 75 Re < 19 + K 0.0033 0.0007 40 Zr < 76 Os < 20 + Ca 0.0058 0.000741 Nb < 77 + Ir 0.021 0.008 21 Sc < 42 Mo < 78 Pt <2e 0.008 22 + Ti0.0028 0.0009 44 Ru < 79 Au < 23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46Pd < 81 Tl < 25 Mn < 47 Ag <2e 0.002 82 Pb < 26 Fe < 48 Cd < 83 Bi < 27Co < 49 In < 90 Th 0.006 0.003 28 Ni < 50 Sn < 92 U < Light ElementsNoble Elements Lanthanides 4 Be 44 Ru < 57 + La 0.016 0.003 5 B 45 Rh <58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e 0.002 60 Nd < 8 O 75 Re < 62Sm < 9 F < 76 Os < 63 Eu < 77 + Ir 0.021 0.008 64 Gd < 78 Pt <2e 0.00865 Tb < 79 Au < 66 Dy < 67 Ho < 68 Er < 69 Tm <2e 0.005 70 Yb < 71 + Lu< KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 102.5%

TABLE 11 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.259 of19-Apr-01 Today 26-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 BOT BOTTOM Further info= 14-01-01 MIDDLE SECTION BOT FACE 4/25/01 Kappa list = 15-Nov-94Channel list = 19-Apr-01 Calculated as: Elements Spectral impurity data:CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = No supporting filmCase number = 0 Known Area, % Rest, Diluent/Sample and Mass/AreaEff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0%Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm < meansthat the concentration is <20 ppm <2e means wt % <2 StdErr. The + in Z +El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt %StdErr Sum Be . . . F 0 0.037 29 + Cu 98.53 0.06 51 Sb < 11 + Na 0.140.01 30 + Zn < 52 Te < 12 Mg <2e 0.004 31 Ga <2e 0.003 53 I < 13 + Al0.78 0.04 32 Ge < 55 Cs < 14 + Si 0.35 0.02 33 As < 56 Ba < 15 + P < 34Se < Sum La . . . Lu 0.024 0.071 16 S 35 Br < 72 + Hf < 16 + So 0.0320.003 37 Rb < 73 + Ta < 17 + Cl 0.061 0.005 38 Sr < 74 W < 18 + Ar 0.0180.002 39 Y < 75 Re < 19 + K 0.021 0.002 40 Zr < 76 Os < 20 + Ca 0.0130.001 41 Nb < 77 + Ir 0.026 0.008 21 Sc < 42 Mo < 78 Pt < 22 Ti <2e0.001 44 Ru < 79 Au < 23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46 Pd < 81Tl < 25 + Mn < 47 Ag < 82 + Pb 0.007 0.003 26 + Fe 0.003 0.001 48 Cd <83 Bi < 27 Co < 49 In < 90 Th <2e 0.003 28 Ni < 50 Sn < 92 U < LightElements Noble Elements Lanthanides 4 Be 44 Ru < 57 La <2e 0.004 5 B 45Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm <9 F < 76 Os < 63 + Eu 0.005 0.002 77 + Ir 0.026 0.008 64 Gd <2e 0.002 78Pt < 65 Tb < 79 Au < 66 Dy < 67 Ho < 68 + Er 0.012 0.004 69 Tm < 70 Yb <71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 102.9%

TABLE 12 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD. 260 of19-Apr-01 Today 26-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 BOT BOTTOM Further info= 14-01-01 MID SECT BOT FACE 4/25/01 BTB Kappa list = 15-Nov-94 Channellist = 19-Apr-01 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be. . . F 0 0.036 29 + Cu 98.55 0.06 51 Sb < 11 + Na 0.12 0.01 30 + Zn <52 Te < 12 Mg <2e 0.004 31 + Ga 0.010 0.003 53 I < 13 + Al 0.77 0.04 32Ge <2e 0.002 55 + Cs 0.006 0.003 14 + Si 0.34 0.02 33 As <2e 0.004 56 Ba0.006 0.003 15 + P < 34 Se < Sum La . . . Lu 0.013 0.071 16 + S 0.0340.003 35 Br < 72 + Hf <2e 0.022 16 So 37 Rb < 73 + Ta < 17 + Cl 0.0640.005 38 Sr < 74 W < 18 + Ar 0.018 0.002 39 Y < 75 Re < 19 + K 0.0210.002 40 Zr < 76 Os <2e 0.007 20 + Ca 0.014 0.001 41 Nb < 77 + Ir 0.0180.007 21 Sc < 42 Mo <2e 0.002 78 Pt < 22 Ti < 44 Ru < 79 + Au 0.0140.007 23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47Ag <2e 0.002 82 Pb <2e 0.003 26 Fe <2e 0.001 48 Cd < 83 + Bi 0.013 0.00527 Co < 49 In < 90 Th <2e 0.003 28 Ni < 50 Sn < 92 U < Light ElementsNoble Elements Lanthanides 4 Be 44 Ru < 57 + La <2e 0.005 5 B 45 Rh < 58Ce <2e 0.002 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e 0.002 60 Nd < 8 O 75 Re <62 Sm < 9 F < 76 Os <2e 0.007 63 Eu < 77 + Ir 0.018 0.007 64 Gd < 78 Pt< 65 Tb <2e 0.002 79 + Au 0.014 0.007 66 Dy < 67 Ho < 68 Er < 69 Tm < 70Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 103.1%

TABLE 13 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.261 of19-Apr-01 Today 26-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-01 BOT BOTTOM Further info= 14-01-01 MID SECT BOT FACE 4/25/01 3 HR Kappa list = 15-Nov-94 Channellist = 19-Apr-01 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff. Diam. =25.00 mm Eff. Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be. . . F 0 0.038 29 + Cu 98.50 0.06 51 Sb < 11 + Na 0.15 0.01 30 + Zn <52 Te < 12 + Mg 0.014 0.004 31 + Ga 0.009 0.003 53 I < 13 + Al 0.79 0.0432 Ge < 55 Cs < 14 + Si 0.35 0.02 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu 0.016 0.071 16 + S 0.036 0.003 35 Br < 72 + Hf < 16 So 37 Rb< 73 + Ta < 17 + Cl 0.062 0.005 38 Sr < 74 W < 18 + Ar 0.018 0.002 39 Y< 75 Re < 19 + K 0.020 0.002 40 Zr < 76 Os < 20 + Ca 0.0108 0.0010 41 Nb< 77 + Ir 0.016 0.007 21 + Sc 0.0020 0.0009 42 Mo < 78 Pt <2e 0.007 22 +Ti <2e 0.001 44 Ru < 79 Au < 23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46Pd < 81 Tl < 25 Mn < 47 Ag <2e 0.002 82 Pb 0.006 0.003 26 Fe <2e 0.00148 + Cd 0.004 0.002 83 Bi < 27 + Co < 49 In < 90 Th <2e 0.003 28 Ni < 50Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La<2e 0.004 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e 0.002 60Nd < 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir 0.016 0.007 64 Gd< 78 Pt <2e 0.007 65 Tb < 79 Au < 66 Dy < 67 Ho < 68 + Er 0.013 0.004 69Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 102.9%

TABLE 14 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.320 of24-May-01 Today 25-May-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-04 Ni AXIAL BLK Furtherinfo = 14-01-04 Ni AXIAL BLK 5/25 Kappa list = 15-Nov-94 Channel list =24-May-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be . . . F 0 0.035 29Cu < 51 Sb < 11 + Na 0.031 0.009 30 Zn < 52 Te < 12 Mg < 31 Ga < 53 I <13 + Al 2.11 0.07 32 Ge < 55 Cs < 14 + Si 0.030 0.005 33 As < 56 Ba <2e0.003 15 + P 0.0020 0.0003 34 Se < Sum La . . . Lu 0.69 1.22 16 S 35 Br< 72 Hf <2e 0.007 16 + So 0.0042 0.0004 37 Rb < 73 + Ta < 17 + Cl < 38Sr < 74 + W < 18 Ar < 39 Y < 75 Re < 19 K < 40 + Zr 0.027 0.002 76 Os <20 Ca < 41 Nb < 77 Ir < 21 + Sc 0.0024 0.0008 42 Mo <2e 0.002 78 Pt < 22Ti < 44 Ru <2e 0.002 79 Au < 23 V < 45 + Rh 0.005 0.002 80 Hg < 24 Cr <46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 Fe < 48 Cd < 83 Bi < 27 Co <49 In < 90 Th < 28 + Ni 97.10 0.08 50 Sn < 92 U < Light Elements NobleElements Lanthanides 4 Be 44 Ru <2e 0.002 57 La < 5 B 45 + Rh 0.0050.002 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm< 9 F < 76 Os < 63 Eu < 77 Ir < 64 Gd < 78 Pt < 65 Tb < 79 Au < 66 + Dy< 67 + Ho < 68 Er < 69 Tm < 70 + Yb 0.69 0.27 71 Lu < KnownConc = 0 REST= 0 D/S = 0Sum Conc's before normalisation to 100%: 101.4%

TABLE 15 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.321 of24-May-01 Today 25-May-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-04 Ni RADIAL BLK Furtherinfo = 14-01-04 Ni RADIAL BLK 5/25 Kappa list = 15-Nov-94 Channel list =24-May-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff. Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be . . . F 0 0.037 29Cu < 51 Sb < 11 + Na 0.12 0.01 30 Zn < 52 Te < 12 Mg < 31 Ga < 53 I <13 + Al 2.57 0.07 32 + Ge 0.005 0.002 55 Cs <2e 0.002 14 + Si 0.14 0.0133 As < 56 Ba 0.006 0.003 15 + P < 34 Se < Sum La . . . Lu 0.65 1.21 16S 35 Br < 72 Hf <2e 0.007 16 + So 0.026 0.002 37 Rb < 73 + Ta < 17 + Cl0.0050 0.0007 38 Sr < 74 + W < 18 + Ar 0.010 0.001 39 Y < 75 Re <2e0.006 19 + K 0.0048 0.0007 40 + Zr 0.032 0.003 76 Os < 20 + Ca 0.0110.001 41 Nb < 77 Ir <2e 0.006 21 Sc < 42 Mo <2e 0.002 78 Pt < 22 Ti < 44Ru < 79 Au < 23 V < 45 Rh < 80 Hg <2e 0.004 24 Cr < 46 Pd < 81 Tl < 25Mn < 47 Ag <2e 0.002 82 Pb < 26 Fe < 48 Cd <2e 0.002 83 Bi < 27 Co < 49In < 90 Th <2e 0.002 28 + Ni 96.43 0.09 50 Sn < 92 U <2e 0.002 LightElements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh < 58Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e 0.002 60 Nd < 8 O 75 Re <2e 0.00662 Sm < 9 F < 76 Os < 63 Eu < 77 Ir <2e 0.006 64 Gd < 78 Pt < 65 Tb <2e0.003 79 Au < 66 + Dy < 67 + Ho < 68 Er < 69 Tm < 70 + Yb 0.64 0.27 71Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 100.5%

TABLE 16 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.327 of1-Jun-01 Today 4-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-05 Co AXIAL TOP Furtherinfo = 14-01-05 CO AXIAL TOP Kappa list = 15-Nov-94 Channel list =24-May-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be . . . F 0 0.88 29Cu < 51 Sb < 11 + Na 0.026 0.008 30 Zn < 52 Te < 12 Mg < 31 Ga <2e 0.00253 I < 13 + Al 4.9 0.1 32 Ge < 55 Cs < 14 + Si 0.073 0.006 33 As < 56 +Ba 0.006 0.003 15 + P 0.0040 0.0004 34 Se < Sum La . . . Lu 0.02 10.0816 S 35 Br < 72 + Hf 0.014 0.006 16 + So < 37 Rb < 73 Ta < 17 + Cl0.0047 0.0006 38 Sr < 74 W < 18 + Ar 0.011 0.001 39 Y < 75 Re < 19 K <40 + Zr 0.019 0.002 76 Os < 20 + Ca 0.0075 0.0007 41 Nb < 77 Ir <2e0.005 21 + Sc 0.0022 0.0006 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79 Au < 23 V< 45 Rh < 80 Hg <2e 0.004 24 Cr < 46 Pd < 81 Tl < 25 + Mn 0.0091 0.000847 Ag < 82 Pb <2e 0.002 26 + Fe 0.13 0.01 48 Cd 0.003 0.002 83 Bi < 27 +Co 94.6 0.1 49 In < 90 Th <2e 0.002 28 + Ni 0.16 0.01 50 Sn < 92 U <Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh< 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm <9 + F < 76 Os < 63 Eu <2e 0.002 77 Ir <2e 0.005 64 + Gd 0.016 0.003 78Pt < 65 Tb < 79 Au < 66 Dy < 67 + Ho < 68 + Er < 69 Tm < 70 + Yb < 71 +Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 102.0%

TABLE 17 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.328 of1-Jun-01 Today 4-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-05 Co RADIAL Further info= 14-01-05 CO RADIAL Kappa list = 15-Nov-94 Channel list = 24-May-01Calculated as: Elements Spectral impurity data: CAL.909 Teflon (7/94)X-ray path = Vacuum Film type = No supporting film Case number = 0 KnownArea, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mm Eff.Area= 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass =18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be . . . F 0 0.88 29Cu < 51 Sb < 11 + Na 0.043 0.009 30 Zn < 52 Te < 12 Mg < 31 Ga < 53 I <13 + Al 3.71 0.09 32 Ge < 55 Cs < 14 + Si 0.18 0.01 33 As < 56 Ba < 15 +P 0.0037 0.0004 34 Se < Sum La . . . Lu 0.02 10.20 16 S 35 Br < 72 Hf<2e 0.006 16 + So < 37 Rb < 73 Ta < 17 + Cl 0.0034 0.0007 38 Sr < 74 W <18 + Ar 0.010 0.001 39 Y < 75 Re <2e 0.005 19 K < 40 + Zr 0.017 0.001 76Os < 20 + Ca 0.0087 0.0008 41 Nb < 77 Ir <2e 0.005 21 + Sc 0.0033 0.000642 Mo < 78 Pt < 22 Ti < 44 Ru <2e 0.002 79 Au < 23 V < 45 Rh <2e 0.00280 Hg <2e 0.004 24 + Cr < 46 Pd < 81 Tl < 25 + Mn 0.0081 0.0007 47 Ag <82 Pb < 26 + Fe 0.13 0.01 48 Cd < 83 Bi < 27 + Co 95.7 0.1 49 In < 90 Th<2e 0.002 28 + Ni 0.18 0.01 50 Sn < 92 U < Light Elements Noble ElementsLanthanides 4 Be 44 Ru <2e 0.002 57 La < 5 B 45 Rh <2e 0.002 58 Ce < 6 C46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re <2e 0.005 62 Sm < 9 + F <76 Os < 63 + Eu 0.008 0.002 77 Ir <2e 0.005 64 + Gd 0.011 0.003 78 Pt <65 Tb < 79 Au < 66 Dy < 67 + Ho < 68 + Er < 69 Tm < 70 + Yb < 71 + Lu <KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 101.3%

TABLE 18 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.330 of4-Jun-01 Today 4-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-06 Cu/Ag/Au AX TOP Furtherinfo = 14-01-06 Cu/Ag/Au AXIAL TOP 6/4/01 Kappa list = 15-Nov-94 Channellist = 4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be. . . F 0 0.041 29 + Cu 96.97 0.09 51 Sb < 11 + Na 0.056 0.010 30 + Zn <52 Te < 12 Mg < 31 + Ga 0.007 0.003 53 I < 13 + Al 0.013 0.003 32 Ge <55 Cs < 14 Si < 33 As < 56 Ba < 15 + P < 34 + Se < Sum La . . . Lu 0.0120.071 16 + S 0.0032 0.0004 35 + Br < 72 + Hf < 16 So 37 + Rb < 73 + Ta <17 + Cl 0.020 0.002 38 Sr < 74 W < 18 + Ar 0.011 0.002 39 Y < 75 + Re0.021 0.008 19 K < 40 + Zr 0.0074 0.0010 76 Os < 20 + Ca 0.0029 0.000841 Nb < 77 + Ir 0.026 0.008 21 + Sc < 42 Mo <2e 0.002 78 Pt < 22 Ti < 44Ru < 79 + Au 1.37 0.05 23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46 Pd < 81Tl < 25 Mn < 47 + Ag 1.49 0.06 82 Pb < 26 Fe < 48 Cd < 83 Bi < 27 Co <49 In < 90 Th <2e 0.003 28 Ni < 50 + Sn < 92 U < Light Elements NobleElements Lanthanides 4 Be 44 Ru < 57 + La <2e 0.004 5 B 45 Rh < 58 Ce <6 C 46 Pd < 59 Pr < 7 N 47 + Ag 1.49 0.06 60 Nd < 8 O 75 + Re 0.0210.008 62 Sm < 9 F < 76 Os < 63 Eu <2e 0.002 77 + Ir 0.026 0.008 64 Gd <78 Pt < 65 Tb <2e 0.002 79 + Au 1.37 0.05 66 Dy < 67 Ho < 68 Er < 69 Tm< 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 100.1%

TABLE 19 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.331 of4-Jun-01 Today 4-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-06 Cu/Ag/Au RADIAL Furtherinfo = 14-01-06 Cu/Ag/Au RADIAL 06/04/01 Kappa list = 15-Nov-94 Channellist = 4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be. . . F 0 0.040 29 + Cu 97.04 0.08 51 Sb < 11 + Na 0.045 0.010 30 + Zn <52 Te < 12 Mg <2e 0.004 31 Ga <2e 0.003 53 I < 13 + Al 0.047 0.004 32 Ge<2e 0.002 55 Cs <2e 0.003 14 Si <2e 0.005 33 As < 56 Ba <2e 0.003 15 + P< 34 + Se < Sum La . . . Lu 0.003 0.071 16 + S 0.0066 0.0006 35 + Br <72 + Hf < 16 So 37 + Rb < 73 + Ta < 17 + Cl 0.025 0.002 38 Sr < 74 W <18 + Ar 0.011 0.002 39 Y < 75 Re <2e 0.008 19 + K 0.0021 0.0008 40 + Zr0.008 0.001 76 Os < 20 + Ca 0.0060 0.0009 41 Nb < 77 + Ir 0.033 0.008 21Sc < 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79 + Au 1.33 0.05 23 V < 45 Rh < 80Hg <2e 0.006 24 + Cr < 46 Pd < 81 Tl < 25 Mn < 47 + Ag 1.44 0.05 82 Pb <26 Fe < 48 Cd < 83 Bi < 27 Co < 49 In < 90 Th < 28 Ni < 50 + Sn < 92 U <Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh< 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 + Ag 1.44 0.05 60 Nd < 8 O 75 Re<2e 0.008 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir 0.033 0.008 64 Gd < 78Pt < 65 Tb <2e 0.002 79 + Au 1.33 0.05 66 Dy < 67 Ho < 68 Er < 69 Tm <70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 100.1%

TABLE 20 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.336 of11-Jun-01 Today 11-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-07 AXIAL Further info =14-01-07 AXIAL LEAD TIN ZINC 6/11 CASS 8 Kappa list = 15-Nov-94 Channellist = 4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be. . . F 0 0.051 29 + Cu 0.24 0.02 51 + Sb 0.023 0.006 11 + Na < 30 + Zn25.4 0.2 52 Te < 12 + Mg 0.016 0.008 31 + Ga < 53 + I <2e 0.82 13 + Al2.08 0.07 32 Ge < 55 Cs < 14 + Si 0.018 0.004 33 As < 56 Ba < 15 + P <34 Se < Sum La . . . Lu 0.035 0.072 16 S 35 Br <2e 0.001 72 Hf < 16 + So0.038 0.003 37 + Rb < 73 Ta < 17 + Cl 0.053 0.004 38 Sr < 74 + W <2e0.012 18 Ar < 39 + Y <2e 0.002 75 Re < 19 K < 40 + Zr 0.024 0.005 76 +Os < 20 + Ca <2e 0.031 41 Nb < 77 + Ir < 21 Sc < 42 Mo < 78 + Pt < 22 Ti< 44 + Ru <2e 0.005 79 Au < 23 V < 45 Rh < 80 Hg < 24 Cr < 46 Pd < 81 +Tl < 25 Mn < 47 Ag < 82 + Pb 16.9 0.2 26 Fe < 48 + Cd 0.014 0.005 83 +Bi < 27 Co <2e 0.001 49 + In <2e 0.011 90 + Th < 28 + Ni 0.007 0.00350 + Sn 54.7 0.2 92 U < Light Elements Noble Elements Lanthanides 4 Be44 + Ru <2e 0.005 57 La < 5 B 45 Rh < 58 + Ce 0.030 0.010 6 C 46 Pd < 59Pr <2e 0.006 7 N 47 Ag < 60 + Nd <2e 0.004 8 O 75 Re < 62 Sm < 9 F <76 + Os < 63 Eu < 77 + Ir < 64 Gd < 78 + Pt < 65 Tb < 79 Au < 66 Dy < 67Ho < 68 Er < 69 Tm < 70 Yb < 71 Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 111.4%

TABLE 21 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.337 of4-Jun-01 Today 11-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-07 RADIAL Further info =14-01-07 RADIAL LEAD/TIN/ZINC 6/11 CS 8 Kappa list = 15-Nov-94 Channellist = 4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0 0.046 29 + Cu 0.014 0.002 51 + Sb 0.015 0.005 11 + Na < 30 + Zn33.2 0.2 52 Te < 12 + Mg < 31 + Ga < 53 + I <2e 0.72 13 + Al 0.17 0.0132 Ge < 55 Cs < 14 + Si 0.026 0.004 33 As < 56 Ba < 15 P < 34 Se < SumLa. . . Lu 0.031 0.069 16 S 35 Br < 72 Hf < 16 + So < 37 + Rb < 73 Ta <17 + Cl 0.031 0.003 38 Sr < 74 + W 0.033 0.014 18 Ar < 39 + Y < 75 Re <19 K < 40 + Zr 0.016 0.005 76 + Os < 20 + Ca <2e 0.027 41 Nb < 77 + Ir <21 Sc < 42 Mo < 78 + Pt < 22 Ti < 44 + Ru 0.011 0.005 79 Au < 23 V < 45Rh < 80 Hg < 24 Cr < 46 Pd < 81 + Tl <2e 0.014 25 Mn < 47 Ag < 82 + Pb18.3 0.2 26 Fe < 48 + Cd 0.025 0.004 83 Bi < 27 Co < 49 + In <2e 0.01090 Th < 28 Ni < 50 + Sn 47.9 0.2 92 U < Light Elements Noble ElementsLanthanides 4 Be 44 + Ru 0.011 0.005 57 La <2e 0.008 5 B 45 Rh < 58 + Ce<2e 0.010 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm < 9F < 76 + Os < 63 Eu < 77 + Ir < 64 Gd <2e 0.004 78 + Pt < 65 Tb < 79 Au< 66 Dy < 67 + Ho 0.012 0.006 68 Er <2e 0.004 69 Tm <2e 0.004 70 Yb <2e0.004 71 Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 115.8%

TABLE 22 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.342 of14-Jun-01 Today 14-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-08 AXIAL Further info =14-01-08 AXIAL Sn, K, Na, Mg 6/14 Kappa list = 15-Nov-94 Channel list =4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.06029 + Cu 0.079 0.006 51 Sb < 11 + Na 1.07 0.05 30 Zn < 52 Te < 12 + Mg0.85 0.04 31 Ga < 53 + I <2e 1.43 13 + Al 1.53 0.06 32 Ge < 55 Cs < 14 +Si 0.16 0.01 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu 0.021 0.07216 S 35 Br < 72 Hf <2e 0.003 16 + So 0.044 0.004 37 Rb < 73 Ta < 17 + Cl0.015 0.001 38 + Sr < 74 + W 0.031 0.004 18 Ar < 39 Y < 75 Re < 19 K <40 + Zr 0.047 0.004 76 Os < 20 + Ca < 41 + Nb < 77 + Ir <2e 0.003 21 +Sc 0.007 0.002 42 Mo < 78 Pt < 22 Ti < 44 + Ru < 79 Au < 23 V <2e 0.00245 Rh < 80 Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 + Pb 0.060.006 26 + Fe 0.017 0.002 48 + Cd 0.041 0.005 83 Bi <2e 0.002 27 + Co0.003 0.001 49 + In <2e 0.019 90 + Th < 28 + Ni 0.021 0.002 50 + Sn 95.60.1 92 U < Light Elements Noble Elements Lanthanides 4 Be 44 + Ru < 57La < 5 B 45 Rh < 58 Ce <2e 0.007 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd<2e 0.005 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir <2e 0.003 64Gd < 78 Pt < 65 Tb < 79 Au < 66 Dy < 67 Ho <2e 0.005 68 Er < 69 Tm <2e0.004 70 Yb < 71 Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 94.8%

TABLE 23 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.343 of4-Jun-01 Today 14-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-01-08 RADIAL Further info =14-01-08 RADIAL Sn, K, Na, Mg 6/14 Kappa list = 15-Nov-94 Channel list =4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.05629 + Cu 0.14 0.01 51 Sb < 11 + Na 2.82 0.08 30 + Zn 0.003 0.002 52 Te <12 + Mg 1.04 0.04 31 Ga < 53 + I <2e 1.40 13 + Al 1.69 0.06 32 Ge < 55Cs < 14 + Si 0.29 0.02 33 As < 56 Ba < 15 + P 0.0022 0.0004 34 Se <SumLa . . . Lu 0.025 0.065 16 S 35 Br < 72 Hf <2e 0.003 16 + So 0.0320.003 37 Rb < 73 Ta < 17 + Cl 0.013 0.001 38 Sr < 74 + W 0.048 0.004 18Ar < 39 Y < 75 Re < 19 K < 40 + Zr 0.043 0.004 76 Os <2e 0.003 20 + Ca <41 + Nb < 77 + Ir <2e 0.003 21 Sc <2e 0.002 42 Mo < 78 Pt < 22 Ti < 44 +Ru < 79 Au < 23 V <2e 0.001 45 Rh < 80 Hg < 24 Cr <2e 0.002 46 Pd < 81 +Tl 0.006 0.003 25 Mn <2e 0.001 47 Ag < 82 + Pb 0.069 0.006 26 + Fe 0.0230.002 48 + Cd 0.029 0.006 83 Bi <2e 0.002 27 Co <2e 0.001 49 + In <2e0.019 90 + Th < 28 + Ni 0.045 0.004 50 + Sn 93.6 0.1 92 U < LightElements Noble Elements Lanthanides 4 Be 44 + Ru < 57 La < 5 B 45 Rh <58 Ce <2e 0.006 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd <2e 0.004 8 O 75Re < 62 Sm <2e 0.005 9 F < 76 Os <2e 0.003 63 Eu <2e 0.004 77 + Ir <2e0.003 64 Gd < 78 Pt < 65 Tb < 79 Au < 66 Dy < 67 Ho < 68 Er < 69 Tm < 70Yb < 71 Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 98.1%

TABLE 24 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.314 of24-May-01 Today 24-May-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-01 Si AXIAL BLK Furtherinfo = 15-01-01 Si AXIAL BLK 5/24 Kappa list = 15-Nov-94 Channel list =24-May-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0.059 0.02129 + Cu 0.012 0.001 51 Sb < 11 + Na 0.004 0.002 30 + Zn 0.0021 0.0005 52Te < 12 Mg < 31 + Ga 0.0038 0.0005 53 I < 13 + Al 1.18 0.05 32 Ge < 55 +Cs <2e 0.003 14 + Si 98.58 0.06 33 As < 56 + Ba 0.008 0.003 15 + P 0.0130.001 34 Se < SumLa . . . Lu 0.004 0.018 16 + S 0.013 0.001 35 Br < 72Hf < 16 So 37 Rb < 73 Ta < 17 + Cl 0.004 0.002 38 Sr < 74 + W 0.0070.001 18 + Ar 0.013 0.003 39 Y < 75 Re < 19 + K < 40 + Zr < 76 Os < 20 +Ca 0.0092 0.0009 41 Nb < 77 Ir < 21 Sc < 42 Mo < 78 Pt < 22 + Ti 0.0190.002 44 Ru < 79 Au < 23 V < 45 Rh < 80 Hg < 24 + Cr 0.0031 0.0005 46 Pd< 81 Tl < 25 + Mn < 47 Ag < 82 Pb < 26 + Fe 0.055 0.005 48 Cd < 83 Bi <27 Co < 49 In < 90 Th < 28 + Ni 0.0051 0.0006 50 Sn < 92 U < LightElements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh < 58Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm < 9 + F0.059 0.021 76 Os < 63 Eu < 77 Ir < 64 Gd < 78 Pt < 65 Tb < 79 Au < 66Dy < 67 Ho < 68 Er < 69 Tm < 70 Yb < 71 Lu < KnownConc = 0 REST = 0 D/S= 0Sum Conc's before normalisation to 100%: 83.4%

TABLE 25 Quantum Catalytics, LLC ANALYSIS REPORT OLD.317 of 24-May-01Today 24-May. Spectrometers configuration: ARL 8410 Rh 60 kV LiF220LiF420 Ge111 TlAP Sample ident = 15-01-01 Si RADIAL BLK Further info =15-01-01 Si RADIAL BLK 5/24 Kappa list = 15-Nov-94 Channel list =24-May-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.02129 + Cu 0.0101 0.0009 51 Sb < 11 + Na 0.016 0.002 30 + Zn 0.0020 0.000552 Te < 12 Mg < 31 + Ga 0.0043 0.0005 53 I < 13 + Al 1.46 0.05 32 Ge <55 + Cs <2e 0.003 14 + Si 98.12 0.07 33 As < 56 + Ba <2e 0.003 15 + P0.018 0.002 34 Se < SumLa . . . Lu 0.005 0.020 16 S 35 Br < 72 + Hf0.003 0.001 16 + So 0.14 0.01 37 Rb < 73 Ta < 17 + Cl 0.019 0.002 38 Sr< 74 + W 0.011 0.001 18 + Ar 0.012 0.003 39 Y < 75 Re < 19 + K 0.0140.001 40 + Zr < 76 Os < 20 + Ca 0.077 0.006 41 Nb < 77 + Ir < 21 Sc < 42Mo < 78 Pt < 22 + Ti 0.029 0.003 44 Ru < 79 Au < 23 + V < 45 Rh < 80 Hg< 24 + Cr 0.0026 0.0005 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 + Fe0.042 0.004 48 Cd < 83 Bi < 27 Co < 49 In < 90 Th < 28 + Ni 0.00530.0006 50 Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44Ru < 57 La < 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd <8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir < 64 Gd <2e 0.001 78Pt < 65 Tb < 79 Au < 66 Dy < 67 Ho < 68 Er < 69 Tm < 70 Yb < 71 Lu <KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 79.7%

TABLE 26 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.237 of23-Apr-01 Today 23-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-01 Si SECTION TOP Furtherinfo = 15-01-01 Si MID SECTION TOP FACE AXIAL Kappa list = 15-Nov-94Channel list = 19-Apr-01 Calculated as: Elements Spectral impurity data:CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = No supporting filmCase number = 0 Known Area, % Rest, Diluent/Sample and Mass/AreaEff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0%Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm < meansthat the concentration is <20 ppm <2e means wt % <2 StdErr. The + in Z +El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt %StdErr SumBe . . . F 0 0.018 29 + Cu 0.0070 0.0006 51 Sb < 11 + Na 0.0500.004 30 + Zn 0.0033 0.0005 52 Te < 12 Mg < 31 + Ga 0.0020 0.0004 53 I <13 + Al 1.02 0.04 32 Ge < 55 Cs <2e 0.003 14 + Si 98.48 0.06 33 As <56 + Ba <2e 0.003 15 + P 0.019 0.002 34 Se < SumLa . . . Lu 0.002 0.01816 + S 0.14 0.01 35 Br < 72 Hf < 16 So 37 Rb < 73 Ta < 17 + Cl 0.0750.006 38 Sr < 74 + W 0.009 0.001 18 + Ar 0.012 0.003 39 Y < 75 Re < 19 +K 0.028 0.002 40 + Zr < 76 Os < 20 + Ca 0.025 0.002 41 Nb < 77 Ir < 21Sc < 42 Mo < 78 Pt < 22 + Ti 0.064 0.005 44 Ru < 79 Au < 23 + V < 45 Rh< 80 Hg < 24 + Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 + Fe0.045 0.004 48 + Cd < 83 Bi < 27 + Co < 49 In < 90 + Th <2e 0.001 28 +Ni 0.0051 0.0006 50 Sn < 92 U < Light Elements Noble ElementsLanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr <7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 Ir < 64Gd < 78 Pt < 65 Tb < 79 Au < 66 Dy < 67 Ho < 68 Er < 69 Tm < 70 Yb < 71Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 90.0%

TABLE 27 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.245 of19-Apr-01 Today 24-Apr-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-01 MID BOTTOM FACE Furtherinfo = 15-01-01 Si MID SECTION BOT FACE AXIAL Kappa list = 15-Nov-94Channel list = 19-Apr-01 Calculated as: Elements Spectral impurity data:CAL.909 Teflon (7/94) X-ray path = Vacuum Film type = No supporting filmCase number = 0 Known Area, % Rest, Diluent/Sample and Mass/AreaEff.Diam. = 25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0%Dil/Sample = 0 Viewed Mass = 18000.00 mg Sample Height = 5 mm < meansthat the concentration is <20 ppm <2e means wt % <2 StdErr. The + in Z +El means involved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt %StdErr SumBe . . . F 0 0.017 29 + Cu 0.0075 0.0007 51 Sb < 11 + Na 0.0330.003 30 + Zn < 52 Te < 12 Mg < 31 + Ga 0.0021 0.0003 53 I < 13 + Al0.71 0.04 32 Ge < 55 + Cs <2e 0.002 14 + Si 98.81 0.05 33 As < 56 + Ba<2e 0.003 15 + P 0.016 0.001 34 Se < SumLa . . . Lu 0.006 0.018 16 + S0.23 0.02 35 Br < 72 Hf < 16 So 37 Rb < 73 Ta < 17 + Cl 0.057 0.005 38Sr < 74 + W 0.007 0.001 18 + Ar 0.007 0.002 39 Y < 75 Re < 19 + K 0.0120.001 40 Zr < 76 Os < 20 + Ca 0.041 0.003 41 Nb < 77 Ir < 21 Sc < 42 Mo< 78 Pt < 22 + Ti 0.020 0.002 44 Ru < 79 Au < 23 + V < 45 Rh < 80 Hg <24 + Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 + Fe 0.026 0.002 48Cd < 83 Bi < 27 + Co < 49 In < 90 Th < 28 + Ni 0.0034 0.0006 50 Sn < 92U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62Sm < 9 F < 76 Os < 63 Eu < 77 Ir < 64 Gd < 78 Pt < 65 Tb < 79 Au < 66 Dy< 67 Ho <2e 0.002 68 + Er <2e 0.001 69 Tm < 70 Yb < 71 Lu < KnownConc =0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 91.9%

TABLE 28 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.326 of1-Jun-01 Today 4-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-02 AXIAL TOP Further info= 15-01-02 AXIAL TOP Kappa list = 15-Nov-94 Channel list = 24-May-01Calculated as: Elements Spectral impurity data: CAL.909 Teflon (7/94)X-ray path = Vacuum Film type = No supporting film Case number = 0 KnownArea, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mm Eff.Area= 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass =18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.02629 + Cu 0.012 0.002 51 Sb < 11 Na <2e 0.009 30 Zn < 52 Te < 12 Mg < 31Ga < 53 I < 13 + Al 1.89 0.06 32 Ge < 55 Cs < 14 + Si 0.032 0.005 33 As< 56 Ba <2e 0.003 15 + P 0.0033 0.0003 34 Se < SumLa . . . Lu 0 0.20 16S 35 Br < 72 Hf <2e 0.005 16 + So 0.0077 0.0007 37 Rb < 73 Ta < 17 + Cl0.0040 0.0006 38 Sr < 74 + W 0.009 0.004 18 + Ar 0.012 0.001 39 Y < 75Re <2e 0.004 19 K < 40 + Zr 0.0099 0.0009 76 Os < 20 + Ca 0.0053 0.000641 Nb < 77 Ir < 21 + Sc 0.0025 0.0005 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79Au < 23 V < 45 Rh < 80 Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag <2e0.002 82 Pb < 26 + Fe 98.01 0.07 48 Cd <2e 0.001 83 Bi < 27 Co < 49 In <90 + Th 0.006 0.002 28 Ni < 50 Sn < 92 U < Light Elements Noble ElementsLanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 + Pr<2e 0.006 7 N 47 Ag <2e 0.002 60 Nd < 8 O 75 Re <2e 0.004 62 + Sm < 9 F< 76 Os < 63 Eu < 77 Ir < 64 Gd < 78 Pt < 65 + Tb < 79 Au < 66 Dy < 67Ho < 68 + Er < 69 + Tm < 70 Yb < 71 Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 96.5%

TABLE 29 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.329 of1-Jun-01 Today 4-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-02 Fe RADIAL Further info= 15-01-02 Fe RADIAL Kappa list = 15-Nov-94 Channel list = 24-May-01Calculated as: Elements Spectral impurity data: CAL.909 Teflon (7/94)X-ray path = Vacuum Film type = No supporting film Case number = 0 KnownArea, % Rest, Diluent/Sample and Mass/Area Eff. Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.02429 + Cu 0.014 0.002 51 Sb < 11 + Na 0.040 0.009 30 Zn < 52 Te < 12 Mg <31 Ga < 53 I < 13 + Al 2.96 0.08 32 Ge < 55 Cs < 14 + Si 0.14 0.01 33 As< 56 Ba < 15 + P 0.0036 0.0003 34 Se < SumLa . . . Lu 0 0.20 16 S 35 Br< 72 Hf < 16 + So 0.012 0.001 37 Rb < 73 Ta < 17 + Cl 0.0044 0.0006 38Sr < 74 W < 18 + Ar 0.013 0.001 39 Y < 75 Re <2e 0.004 19 K < 40 + Zr0.012 0.001 76 Os < 20 + Ca 0.0073 0.0007 41 Nb < 77 Ir < 21 + Sc 0.00260.0005 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79 Au < 23 V < 45 Rh < 80 Hg <2e0.003 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 + Fe 96.78 0.0948 Cd < 83 Bi < 27 Co < 49 In < 90 Th <2e 0.002 28 Ni < 50 Sn < 92 U <Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh< 58 Ce <2e 0.003 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re <2e0.004 62 + Sm < 9 F < 76 Os < 63 Eu <2e 0.003 77 Ir < 64 Gd < 78 Pt <65 + Tb < 79 Au < 66 Dy < 67 Ho < 68 + Er < 69 + Tm < 70 Yb < 71 Lu <KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 97.8%

TABLE 30 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.338 of11-Jun-01 Today 11-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-04 AXIAL Further info =15-01-04 Ni/W/Ta/Hf AXIAL 6/11 Kappa list = 15-Nov-94 Channel list =4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.036 29Cu < 51 Sb < 11 + Na 0.066 0.009 30 Zn < 52 Te < 12 Mg < 31 Ga < 53 I <13 + Al 3.57 0.09 32 Ge < 55 Cs < 14 + Si 0.23 0.02 33 As < 56 Ba < 15 +P 0.0025 0.0004 34 + Se < SumLa . . . Lu 0.58 1.17 16 + S 0.0069 0.000635 Br < 72 + Hf 1.78 0.06 16 So 37 Rb < 73 + Ta 1.76 0.06 17 + Cl 0.00440.0008 38 Sr < 74 + W 1.49 0.06 18 + Ar 0.018 0.002 39 Y < 75 Re < 19 K< 40 + Zr < 76 Os < 20 + Ca 0.0025 0.0008 41 Nb < 77 + Ir < 21 + Sc0.0036 0.0009 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79 Au < 23 V < 45 Rh <80 + Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 Fe < 48 Cd< 83 + Bi < 27 Co < 49 In < 90 Th <2e 0.003 28 + Ni 90.5 0.1 50 Sn < 92U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62Sm < 9 F < 76 Os < 63 Eu <2e 0.002 77 + Ir < 64 Gd < 78 Pt < 65 Tb < 79Au < 66 Dy < 67 + Ho < 68 + Er < 69 + Tm < 70 + Yb 0.58 0.26 71 Lu <KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 101.0%

TABLE 31 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.339 of4-Jun-01 Today 11-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-04 RADIAL Further info =15-01-04 Ni/W/Ta/Hf RADIAL 6/11 Kappa list = 15-Nov-94 Channel list =4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.03629 + Cu < 51 Sb < 11 + Na 0.043 0.009 30 Zn < 52 Te < 12 Mg < 31 + Ga<2e 0.002 53 I < 13 + Al 3.38 0.09 32 + Ge < 55 Cs <2e 0.003 14 + Si0.74 0.04 33 As < 56 Ba < 15 + P < 34 + Se < SumLa . . . Lu 0.57 1.1616 + S 0.0053 0.0005 35 Br < 72 + Hf 2.00 0.07 16 So 37 Rb < 73 + Ta1.78 0.06 17 + Cl 0.0059 0.0008 38 Sr < 74 + W 1.50 0.06 18 + Ar 0.0190.002 39 Y < 75 + Re < 19 K < 40 + Zr < 76 Os < 20 Ca < 41 Nb < 77 + Ir< 21 + Sc 0.0020 0.0009 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79 + Au < 23 V <45 Rh < 80 + Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 Fe< 48 Cd <2e 0.002 83 + Bi < 27 Co < 49 In < 90 Th <2e 0.003 28 + Ni 90.00.2 50 Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru< 57 La < 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8O 75 + Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir < 64 Gd <2e 0.002 78Pt < 65 Tb < 79 + Au < 66 Dy < 67 + Ho < 68 + Er < 69 + Tm < 70 + Yb0.57 0.26 71 Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 101.9%

TABLE 32 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.615 of7-Mar-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-00-01 AX Further info =14-00-01 AXIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list =8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.04329 + Cu 98.88 0.05 51 Sb < 11 + Na 0.063 0.012 30 + Zn < 52 Te < 12 Mg <31 + Ga 0.008 0.003 53 I < 13 + Al 0.33 0.02 32 Ge < 55 Cs < 14 + Si0.66 0.03 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu 0.021 0.07316 + S 0.0042 0.0004 35 Br < 72 + Hf < 16 So 37 Rb < 73 + Ta < 17 + Cl0.026 0.002 38 Sr < 74 W < 18 + Ar 0.013 0.001 39 Y < 75 Re < 19 K < 40Zr < 76 Os < 20 Ca < 41 Nb < 77 Ir <2e 0.008 21 + Sc < 42 Mo <2e 0.00278 Pt < 22 Ti < 44 Ru < 79 Au < 23 V < 45 Rh <2e 0.002 80 Hg <2e 0.00624 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag <2e 0.002 82 Pb < 26 Fe < 48 Cd<2e 0.002 83 Bi < 27 Co < 49 In < 90 Th < 28 Ni < 50 Sn < 92 U < LightElements Noble Elements Lanthanides 4 Be 44 Ru < 57 + La 0.012 0.005 5 B45 Rh <2e 0.002 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e 0.002 60 Nd <8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 Ir <2e 0.008 64 Gd < 78 Pt< 65 Tb <2e 0.002 79 Au < 66 Dy < 67 Ho < 68 Er <2e 0.004 69 Tm <2e0.004 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 100.0%

TABLE 33 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.620 of8-Jan-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-00-01 RAD Further info =14-00-01 RADIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list= 8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0.11 0.04 29 + Cu 98.84 0.05 51 Sb < 11 + Na 0.11 0.01 30 + Zn <52 Te < 12 Mg < 31 Ga <2e 0.003 53 I < 13 + Al 0.28 0.02 32 Ge < 55 Cs<2e 0.003 14 + Si 0.58 0.03 33 As < 56 Ba 0.006 0.003 15 + P < 34 Se <SumLa . . . Lu 0.011 0.072 16 + S 0.0065 0.0006 35 Br < 72 + Hf < 16 So37 Rb < 73 + Ta < 17 + Cl 0.029 0.002 38 Sr < 74 W < 18 + Ar 0.015 0.00139 Y < 75 Re <2e 0.007 19 + K 0.0021 0.0007 40 Zr < 76 Os <2e 0.007 20 +Ca 0.0041 0.0008 41 Nb < 77 + Ir 0.018 0.008 21 Sc < 42 + Mo <2e 0.00278 Pt <2e 0.008 22 Ti <2e 0.001 44 Ru <2e 0.002 79 Au < 23 V < 45 Rh <80 Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag <2e 0.002 82 Pb < 26 Fe <48 Cd <2e 0.002 83 Bi < 27 + Co < 49 In < 90 Th <2e 0.003 28 Ni < 50 Sn< 92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru <2e 0.00257 La <2e 0.005 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag <2e0.002 60 Nd < 8 O 75 Re <2e 0.007 62 Sm < 9 + F 0.11 0.04 76 Os <2e0.007 63 Eu <2e 0.002 77 + Ir 0.018 0.008 64 Gd < 78 Pt <2e 0.008 65 Tb<2e 0.002 79 Au < 66 Dy < 67 Ho < 68 Er < 69 Tm <2e 0.004 70 Yb < 71 +Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 99.8%

TABLE 34 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.613 of7-Mar-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-00-03 AX Further info =14-00-03 AXIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list =8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.04329 + Cu 99.69 0.03 51 Sb < 11 + Na 0.039 0.012 30 + Zn < 52 Te < 12 Mg <31 Ga <2e 0.003 53 I < 13 + Al 0.103 0.008 32 Ge <2e 0.002 55 Cs < 14 +Si 0.036 0.006 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu 0.0330.071 16 + S 0.0056 0.0005 35 Br < 72 + Hf < 16 So 37 Rb < 73 + Ta <17 + Cl 0.037 0.003 38 Sr < 74 W < 18 + Ar 0.013 0.001 39 Y < 75 Re <19 + K < 40 Zr < 76 Os < 20 + Ca 0.0048 0.0008 41 Nb < 77 + Ir 0.0310.008 21 Sc < 42 + Mo 0.005 0.002 78 Pt < 22 + Ti 0.003 0.001 44 Ru < 79Au <2e 0.007 23 V < 45 Rh < 80 Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47Ag < 82 Pb < 26 Fe < 48 Cd <2e 0.002 83 Bi < 27 + Co < 49 In < 90 Th <28 Ni < 50 Sn < 92 U < Light Elements Noble Elements Lanthanides 4 Be 44Ru < 57 + La 0.015 0.005 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47Ag < 60 Nd < 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu <2e 0.002 77 + Ir0.031 0.008 64 Gd < 78 Pt < 65 Tb < 79 Au <2e 0.007 66 Dy < 67 Ho < 68 +Er 0.015 0.004 69 Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 99.4%

TABLE 35 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.618 of8-Jan-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-00-03 RAD Further info =14-00-03 RADIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list= 8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0 0.042 29 + Cu 98.93 0.05 51 Sb < 11 + Na 0.23 0.02 30 + Zn < 52Te < 12 Mg < 31 + Ga 0.008 0.003 53 I < 13 + Al 0.37 0.02 32 Ge <2e0.003 55 Cs < 14 + Si 0.29 0.02 33 As < 56 Ba < 15 + P 0.004 0.001 34 Se< SumLa . . . Lu 0.008 0.072 16 + S 0.021 0.002 35 Br < 72 + Hf < 16 So37 Rb < 73 + Ta < 17 + Cl 0.068 0.006 38 Sr <2e 0.001 74 W < 18 + Ar0.018 0.002 39 Y < 75 Re < 19 + K 0.013 0.001 40 Zr < 76 Os < 20 + Ca0.017 0.002 41 Nb < 77 + Ir 0.023 0.008 21 + Sc 0.0036 0.0009 42 Mo < 78Pt < 22 Ti < 44 Ru < 79 Au < 23 V < 45 Rh <2e 0.002 80 Hg <2e 0.007 24Cr < 46 Pd < 81 Tl <2e 0.005 25 Mn < 47 + Ag 0.004 0.002 82 Pb <2e 0.00326 Fe < 48 Cd <2e 0.002 83 Bi < 27 Co < 49 In < 90 Th < 28 Ni < 50 Sn <92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5B 45 Rh <2e 0.002 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 + Ag 0.004 0.002 60Nd < 8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir 0.023 0.008 64 Gd< 78 Pt < 65 Tb <2e 0.002 79 Au < 66 Dy < 67 Ho < 68 Er <2e 0.004 69 Tm< 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 90.0%

TABLE 36 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.612 of7-Mar-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-00-04 AX Further info =14-00-04 AXIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list =8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.04229 + Cu 99.29 0.05 51 Sb < 11 + Na 0.070 0.011 30 + Zn < 52 Te < 12 Mg <31 Ga <2e 0.003 53 I < 13 + Al 0.27 0.02 32 Ge < 55 Cs <2e 0.003 14 + Si0.29 0.02 33 As < 56 Ba <2e 0.003 15 + P < 34 Se < SumLa . . . Lu 0.0230.072 16 S 35 Br < 72 + Hf <2e 0.022 16 + So 0.0074 0.0007 37 Rb < 73 +Ta < 17 + Cl 0.021 0.002 38 Sr < 74 W < 18 + Ar 0.012 0.001 39 Y < 75 Re< 19 + K 0.0023 0.0007 40 Zr < 76 Os < 20 Ca < 41 Nb < 77 + Ir 0.0260.008 21 Sc < 42 Mo < 78 Pt <2e 0.007 22 + Ti <2e 0.001 44 Ru < 79 Au <23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag <82 Pb < 26 Fe < 48 Cd < 83 Bi < 27 Co < 49 In < 90 Th < 28 Ni < 50 Sn <92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 + La0.013 0.005 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd <8 O 75 Re < 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir 0.026 0.008 64 Gd < 78Pt <2e 0.007 65 Tb <2e 0.002 79 Au < 66 Dy < 67 Ho < 68 Er <2e 0.004 69Tm <2e 0.004 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 99.5%

TABLE 37 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.619 of8-Jan-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 14-00-04 RAD Further info =14-00-04 RADIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list= 8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0 0.044 29 + Cu 98.59 0.06 51 Sb < 11 + Na 0.062 0.012 30 + Zn <52 Te < 12 Mg < 31 Ga <2e 0.003 53 I < 13 + Al 0.63 0.03 32 Ge < 55 Cs <14 + Si 0.60 0.03 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu 0.0210.073 16 + S 0.012 0.001 35 Br < 72 + Hf <2e 0.022 16 So 37 Rb < 73 + Ta< 17 + Cl 0.020 0.002 38 Sr < 74 W < 18 + Ar 0.016 0.002 39 Y < 75 Re<2e 0.009 19 + K < 40 + Zr 0.005 0.001 76 Os < 20 + Ca 0.0109 0.0010 41Nb < 77 + Ir 0.035 0.009 21 Sc < 42 Mo < 78 Pt < 22 + Ti 0.0037 0.001044 Ru <2e 0.002 79 Au < 23 V < 45 Rh < 80 Hg <2e 0.006 24 + Cr 0.00200.0006 46 Pd < 81 Tl < 25 Mn < 47 Ag < 82 Pb < 26 Fe < 48 Cd <2e 0.00283 Bi < 27 Co < 49 In < 90 Th <2e 0.003 28 Ni < 50 Sn < 92 U < LightElements Noble Elements Lanthanides 4 Be 44 Ru <2e 0.002 57 + La 0.0100.004 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr 0.005 0.002 7 N 47 Ag < 60Nd < 8 O 75 Re <2e 0.009 62 Sm < 9 F < 76 Os < 63 Eu < 77 + Ir 0.0350.009 64 Gd <2e 0.002 78 Pt < 65 Tb <2e 0.002 79 Au < 66 Dy < 67 Ho < 68Er < 69 Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 88.1%

TABLE 38 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.614 of7-Mar-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-00-01 AX Further info =15-00-01 AXIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list =8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.04329 + Cu 99.21 0.04 51 Sb < 11 + Na 0.048 0.012 30 + Zn < 52 Te < 12 Mg <31 + Ga 0.008 0.003 53 I < 13 + Al 0.29 0.02 32 Ge <2e 0.002 55 Cs <2e0.003 14 + Si 0.37 0.02 33 As < 56 Ba < 15 + P < 34 Se < SumLa . . . Lu0.011 0.072 16 + S 0.0043 0.0004 35 Br < 72 + Hf <2e 0.022 16 So 37 Rb <73 + Ta < 17 + Cl 0.021 0.002 38 Sr < 74 W < 18 + Ar 0.014 0.001 39 Y <75 Re <2e 0.008 19 + K < 40 Zr < 76 Os <2e 0.007 20 Ca < 41 Nb < 77 + Ir0.036 0.008 21 + Sc 0.0021 0.0009 42 Mo < 78 Pt < 22 Ti < 44 Ru < 79 Au<2e 0.007 23 V < 45 Rh < 80 Hg < 24 Cr < 46 Pd < 81 Tl < 25 Mn < 47 Ag <82 Pb < 26 Fe < 48 Cd < 83 Bi < 27 Co < 49 In < 90 Th < 28 Ni < 50 Sn <92 U < Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La <2e0.005 5 B 45 Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75Re <2e 0.008 62 Sm < 9 F < 76 Os <2e 0.007 63 Eu < 77 + Ir 0.036 0.00864 Gd < 78 Pt < 65 Tb < 79 Au <2e 0.007 66 Dy < 67 Ho < 68 Er <2e 0.00469 Tm < 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 99.7%

TABLE 39 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.617 of8-Jan-02 Today 7-Mar-02 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-00-01 RAD Further info =15-00-01 RADIAL POLISHED VAC 3/7/02 Kappa list = 15-Nov-94 Channel list= 8-Jan-02 Calculated as: Elements Spectral impurity data: CAL.909Teflon (7/94) X-ray path = Vacuum Film type = No supporting film Casenumber = 0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. =25.00 mm Eff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0Viewed Mass = 18000.00 mg Sample Height = 5 mm < means that theconcentration is <20 ppm <2e means wt % <2 StdErr. The + in Z + El meansinvolved in Sum = 100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe .. . F 0 0.041 29 + Cu 99.39 0.05 51 Sb < 11 + Na 0.093 0.012 30 + Zn <52 Te < 12 Mg < 31 + Ga 0.007 0.003 53 I < 13 + Al 0.33 0.02 32 Ge <2e0.002 55 Cs < 14 + Si 0.068 0.006 33 As < 56 Ba < 15 + P < 34 Se < SumLa. . . Lu 0.017 0.073 16 + S 0.0083 0.0007 35 Br < 72 + Hf < 16 So 37 Rb< 73 + Ta < 17 + Cl 0.034 0.003 38 Sr < 74 W < 18 + Ar 0.017 0.002 39 Y< 75 Re < 19 + K 0.0053 0.0008 40 Zr < 76 Os < 20 + Ca 0.0036 0.0008 41Nb < 77 + Ir 0.031 0.008 21 Sc < 42 Mo <2e 0.002 78 Pt < 22 Ti < 44 Ru<2e 0.002 79 Au <2e 0.007 23 V < 45 Rh < 80 Hg <2e 0.006 24 Cr < 46 Pd <81 + Tl 0.014 0.005 25 Mn < 47 Ag < 82 Pb < 26 Fe < 48 Cd < 83 Bi <2e0.005 27 Co < 49 In < 90 Th < 28 Ni < 50 Sn < 92 U < Light ElementsNoble Elements Lanthanides 4 Be 44 Ru <2e 0.002 57 La <2e 0.005 5 B 45Rh < 58 Ce < 6 C 46 Pd < 59 Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 Sm <9 F < 76 Os < 63 Eu <2e 0.002 77 + Ir 0.031 0.008 64 Gd <2e 0.002 78 Pt< 65 Tb < 79 Au <2e 0.007 66 Dy < 67 Ho < 68 Er <2e 0.004 69 Tm <2e0.004 70 Yb < 71 + Lu < KnownConc = 0 REST = 0 D/S = 0Sum Conc's before normalisation to 100%: 94.6%

TABLE 40 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.340 of11-Jun-01 Today 11-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-03 AXIAL Further info =15-01-03 AXIAL Fe, Cr, Mn, V 6/11 Kappa list = 15-Nov-94 Channel list =4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr SumBe . . . F 0 0.03929 + Cu 0.028 0.002 51 Sb < 11 + Na 0.032 0.009 30 + Zn 0.005 0.002 52Te < 12 Mg < 31 Ga <2e 0.001 53 I <2e 0.002 13 + Al 2.28 0.07 32 Ge < 55Cs <2e 0.002 14 Si < 33 As < 56 + Ba <2e 0.003 15 + P 0.0038 0.0003 34Se < SumLa . . . Lu 0 0.21 16 S 35 Br < 72 Hf <2e 0.004 16 + So 0.00920.0008 37 Rb < 73 Ta < 17 + Cl 0.017 0.002 38 Sr < 74 W <2e 0.004 18 +Ar 0.009 0.001 39 Y < 75 Re < 19 + K < 40 + Zr 0.045 0.004 76 Os < 20 +Ca 0.0060 0.0006 41 Nb < 77 Ir < 21 Sc < 42 Mo < 78 Pt < 22 Ti < 44 Ru <79 Au < 23 + V 2.38 0.07 45 Rh < 80 Hg < 24 + Cr 2.71 0.08 46 Pd < 81 Tl< 25 + Mn 2.05 0.07 47 Ag < 82 Pb < 26 + Fe 90.4 0.1 48 Cd < 83 Bi < 27Co < 49 In < 90 + Th 0.005 0.002 28 + Ni 0.012 0.003 50 Sn < 92 U <Light Elements Noble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh< 58 Ce < 6 C 46 Pd < 59 + Pr < 7 N 47 Ag < 60 Nd < 8 O 75 Re < 62 + Sm< 9 F < 76 Os < 63 + Eu < 77 Ir < 64 Gd < 78 Pt < 65 + Tb < 79 Au < 66Dy < 67 Ho < 68 + Er < 69 + Tm < 70 Yb < 71 Lu < KnownConc = 0 REST = 0D/S = 0Sum Conc's before normalisation to 100%: 100.1%

TABLE 41 Quantum Catalytics, LLC ANALYSIS REPORT by Uniquant OLD.341 of4-Jun-01 Today 11-Jun-01 Spectrometers configuration: ARL 8410 Rh 60 kVLiF220 LiF420 Ge111 TlAP Sample ident = 15-01-03 RADIAL Further info =15-01-03 RADIAL Fe, Cr, Mn, V 6/11 Kappa list = 15-Nov-94 Channel list =4-Jun-01 Calculated as: Elements Spectral impurity data: CAL.909 Teflon(7/94) X-ray path = Vacuum Film type = No supporting film Case number =0 Known Area, % Rest, Diluent/Sample and Mass/Area Eff.Diam. = 25.00 mmEff.Area = 490.6 mm2 KnownConc = 0% Rest = 0% Dil/Sample = 0 Viewed Mass= 18000.00 mg Sample Height = 5 mm < means that the concentration is <20ppm <2e means wt % <2 StdErr. The + in Z + El means involved in Sum =100% Z wt % StdErr Z wt % StdErr Z wt % StdErr Sum Be . . . F 0 0.03629 + Cu 0.16 0.01 51 Sb < 11 + Na 0.083 0.009 30 + Zn 0.032 0.003 52 Te< 12 + Mg 0.013 0.003 31 Ga <2e 0.001 53 I < 13 + Al 4.5 0.1 32 Ge < 55Cs < 14 + Si 0.15 0.01 33 As < 56 Ba < 15 + P 0.0097 0.0009 34 Se <SumLa . . . Lu 0 0.20 16 S 35 Br < 72 + Hf 0.018 0.004 16 + So 0.0480.004 37 Rb < 73 Ta < 17 + Cl 0.032 0.003 38 Sr < 74 + W 0.008 0.00418 + Ar 0.010 0.001 39 Y < 75 Re < 19 + K 0.019 0.002 40 + Zr 0.0970.008 76 Os < 20 + Ca 0.051 0.004 41 Nb < 77 Ir <2e 0.003 21 Sc < 42 Mo<2e 0.002 78 Pt < 22 + Ti 0.0030 0.0006 44 Ru < 79 Au < 23 + V 2.26 0.0745 Rh < 80 Hg < 24 + Cr 2.39 0.07 46 Pd < 81 Tl < 25 + Mn 2.20 0.07 47Ag <2e 0.001 82 Pb < 26 + Fe 87.9 0.2 48 Cd <2e 0.001 83 Bi < 27 Co < 49In < 90 + Th 0.006 0.002 28 Ni <2e 0.003 50 Sn < 92 U < Light ElementsNoble Elements Lanthanides 4 Be 44 Ru < 57 La < 5 B 45 Rh < 58 Ce < 6 C46 Pd < 59 + Pr < 7 N 47 Ag <2e 0.001 60 Nd < 8 O 75 Re < 62 + Sm < 9 F< 76 Os < 63 + Eu < 77 Ir <2e 0.003 64 Gd < 78 Pt < 65 + Tb < 79 Au < 66Dy < 67 Ho < 68 + Er < 69 + Tm < 70 Yb < 71 Lu < KnownConc = 0 REST = 0D/S = 0Sum Conc's before normalisation to 100%: 99.9%

1. A method of processing copper, comprising: (1.) contacting moltencopper with a carbon source; (2.) an iterative cycling process, whereinrelative saturation of copper with carbon remains the same or increasesindependently with each cycle; and (3.) cooling the molten copper toroom temperature, thereby obtaining a solidified manufactured copper.